Here's a list of places in and around Grand Central Station that sells the $4 fun pass:
http://www.mta.nyc.ny.us/metrocard/mcml/4funpmn3.htm
The express bus stops on Park Ave, just South of 42nd St. Walk North, cross 42nd St, and enter Grand Central. I believe that the newstand inside the door of Grand Central is one of the newstands in the listings. If not there are several others. You can ask at the NYC TA info booth in the middle of the lobby inside Grand Central.
-David
Edited to note that the express bus stop is just South of 42nd Street (Not North).
[This message has been edited by LIH Prem (edited 04-30-2001).]