Looking for another great neighborhood to stay
 

The last three times we have visited Tokyo, we have stayed at either the Hilton or Park Hyatt Shinjuku. While we really don't love the busy Shinjuku area, we love the location of these hotels. They both offer free bike rentals, and we enjoy riding our bikes from Shinjuku to Shibuya to Kitazawa, to Ebisu, etc. You go from a nice busy hub around the train station and then bike through beautiful parks and quaint neighborhoods until you get to the next cool busy hub to walk around.

This time, we would like to explore a different area of Tokyo, but still do it by bicycle (we are very comfortable on bikes in Tokyo and have biked hundreds of miles through the city). We like to bike from a cool central hood, get off our bikes and walk around for a few hours (kitazawa is a good example), and then get on our bikes and stroll to the next cool neighborhood where we can get off and walk around/shop/explore.

Does anyone have any other suggestions for this? Would be great to be in a totally different area of Tokyo!

How about around Iidabashi? Nice green along the river south (dont know if bikes are allowed there). Ueno park or Koishikawa Korakuen Gardens not far..

Hotels - many, if not "must be chain" :)

You're basically looking for interesting walkable neighbourhoods that are in reasonable proximity from one another so that you can hop in between by bike, correct?

The area that comes to mind immediately would be Shibuya as the base from which there are interesting neighborhood to the south (Daikanyama, Nakameguro), west (Shimokitazawa, Sankenjaya), north (Harajuku) and east (Aoyama). Further down along Toyoko line, you've got Jiyugaoka which great... I am partial to Setagaya-ku and beyond, heading down towards Yokohama.

Unfortunately Jiyugaoka itself lacks great hotel options, and I'm not sure if there are good hotels somewhere between Jiyugaoka and Shibuya. But the advantage of staying around the area between Shibuya and Tamagawa (Tama River) would be that you'll have access to Tamagawa cycling road which goes all the way to near Yokota AFB, in addition to being able to access all the aforementioned neighborhoods even though Shibuya would still be a lot more central.

Futako Tamagawa is an awesome area with a good hotel (Tokyu Excel) and a huge shopping center, although I'm not sure you'd be into that and it is a bit out of the way with respect to those other neighborhoods if you're going to be biking.

If you just want to be able to ride bike but then you are okay with relying on trains to see places, then Tachikawa is a good option. Tachikawa itself has tons of food and shopping, you have easy access to Tamagawa's cycling road, there are many great parks and semi-nature areas nearby, plus you can probably bike to Kichijoji which is an amazing area to explore.

I know you're looking for recommendations in Tokyo but Kyoto and Nara are also great cities to explore on two wheels.

Oh alright. Back to Tokyo ... With the sharing scheme, you can pick up e-bikes in just about any part of central Tokyo, so you could get a bus or train to a neighborhood that you want to explore and go pick up a bike in situ.
https://docomo-cycle.jp/tokyo-project/en_index.html

For pleasant areas to explore on bicycles I'd suggestL
Ueno / Yanasen neighborhoods
Iidabashi / Yotsuya / Yasukuni jinja etc. (already proposed above)
Shinjuku Gyoen / Sendagaya / Harajuku / Meiji jingu
Hibiya / Marunouchi / Ginza
Ryogoku / Sumida river / Asakusa

The bike scheme doesn't appear to extend to outer Tokyo wards like Katsushika yet. Perhaps you can find bike rental out there ... It could be quite nice to explore that old-world neighborhood and then ride along the banks of the Edo river.

EDIT: For Shibamata and Edo river you can rent bicycles from Shibamata at 400 yen per day:
http://www.katsushika-kanko.com/rental-bicycle/

Heartily agree. Have you travelled much outside of Tokyo?

Thanks guys. On this trip we are doing Osaka and Kyoto for the first time as well. We have bike rentals arranged for our entire stay. We are in the Kita neighborhood in Osaka (Intercontinental), and we are right by Nishiki Market in Kyoto.

Your first sentence nails my request, much more eloquently. Thank you. We have done Shibuya/surrounding hoods, so I think that is a great suggestion, but would like to stray further from that area. I am going to take a look at Setagaya-ku and beyond. We really love wandering cool areas. We absolutely loved wandering the streets of Shimokitazawa, and we really enjoyed walking from Shibuya to Harajuku on the streets slightly East of the train line. Would be looking to land at neighborhoods like that on our next adventure.

Just to clarify, Setagaya-ku is a precinct with cachet as a desirable place to live but probably would not interest most visitors, generally speaking. I only brought it up because I raved about Jiyugaoka but with caviat that I personally love Setagaya-ku (which Jiyugaoka is part of). Having said that, there are some neighbourhoods within Setagaya-ku that I think you'd enjoy such as Jiyugaoka and Sangenjaya. Moreover you'll be relatively close to Tamagawa (Tama River) and its trail. Have you been to Sangenjaya, Kichijoji and Nakameguro? If you enjoy Japanese shopping arcades/streets, Kichijoji, Asagaya and Nakano all have good ones and they're all close to each other.

You took my two best ideas so I'll just say +1. Both areas are great for walking and site-seeing.

Amazing. Thanks so much. This gives me a good idea where to base out of now! The Aman seems pretty close...

They're great areas to explore. They're also popular bases for more budget conscious tourists, but AFAIK there's no deluxe hotel around Ueno / Yanasen / Ryogoku etc. I saw that you previously stayed at the Park Hyatt - so that's why I thought you might prefer to commute by train from a more upscale neighbourhood. If you wanted to, though, you could get a suite at the Nohga Ueno for a similar price to a regular room at a deluxe property. I wouldn't expect the same level of service, but the suite looks very nice, it has bicycles for rent, and it's minutes from Ueno station. (And from Keisei Ueno, you have the fastest connection to Narita Airport, which can be useful).
https://nohgahotel.com/en/ueno/rooms/

Can I ask you OP when you travel to the Tokyo area? I've been keen on using a bike more in Tokyo but I've not been successful- mostly due to clothing and weather constraints. What time of the year are you travelling?
Do you use a basket or a pannier?
For me, I sweat buckets biking in the pacific north west where its perfect biking weather, so I worry I'll just be a perpetual puddle biking around Tokyo between May-Sep.
What type of bike are you using?

It's too late for this trip but for next time, may I suggest central Yokohama. There are at least two days worth of things to explore, plus Kamakura (you might want to rent bikes there rather than bike there from Yokohama) and the cute coastal towns in that area.

From Kamakura most convenient way to get to coastal area is to take Enoden (cannot use JR pass) which runs between Kamakura and Fujisawa. The train will take you to coastal area of Enoshima. Enoshima (island) itself is a nice place to visit, connected by a bridge between main land.

For other coastal area from Kamakura will be by bus, which can be less frequent than Enoden and during weekends and during rush hours buses can be slow going in the traffic.

P.S.
Alright, you can take JR Yokosuka Line from Kamakura to Yokosuka and Kurihama, both are coastal city. From Kurihama one can take a ferry to cross Tokyo Bay to Boso peninsula to Kanaya. :)