Take this with a grain of salt as I've never stayed at Jersey City, but if you are coming from EWR and spending your time in the city, it seems like its going to be a pain to get to. Wouldn't you have to take NJ Transit from EWR to Penn and then PATH back out to Jersey City?
I've stayed at most of the NYC properties, except for the PH, Union Square, and Times Square. P+C availability can be really hard to find in my experience, thus the reason I haven't stayed at Union Square.
If you are looking for a place to sleep and will be enjoying the city, vs trying to find a top notch full service hotel to spend the time in, I'd actually suggest either Herald Square or the Hyatt Place Midtown South. I've done a few stays this year at Herald Sq. primarily due to the convenience to Penn Station, but couldn't get P+C availability last week and ended up at the HP.
I was actually very pleasantly surprised by the HP. Granted that I spent the vast majority of my time out of the hotel, and noticed that the breakfast area was a mad house on the Sunday morning I was there. But, for me, its NYC, there's no way I'd choose a HP breakfast over a good diner or bagel.
All in all, my thought process in NYC is mainly around where you want to be in town.
I find the GH too big and too busy and the rooms are old. Usually not worth the price for me unless I happen to be going in/out of Grand Central which is rare.
The Andaz 5th Ave is nice, but I haven't stayed since they first opened so my data is old. Its great being next to Bryant Park though
Andaz Wall St is fine, but too far out of the way for me in most cases to win out.
Since I've been doing quick 1 day trips using Penn to get to/from either JFK or EWR or Amtrak lately, I've been aiming for the properties around there and as much as I like the Union Square area, either Herald Sq or HP Midtown/South are much better location wise and subway access wise to the places in the city that I spend my time.
On a side note, if you are looking for food, I had dinner at Union Square Café last week and it was out of this world excellent. Enjoy!