Those are two really different places that offer very different lifestyles and I find it hard to imagine being really interested in both. We looked at both, but were quickly able to rule one out. I wouldn't move to Croton just for a bigger house or lot. You should consider Croton if you're interested in what it offers--a pleasant town surrounded by lovely natural beauty, great parks on the Hudson, nice hiking trails through the woods, easy access to a great number of nature reserves and parks with tremendous opportunites for outdoor activities, an easy commute (trains are very frequent and express trains are 43 to 48 minutes to GC), and good schools. Within the Croton school district, you can get a house in the village center within walking distance to schools, parks, and amenities--or you can get a house outside of the center in a "country" setting with land and privacy. Croton has a nice range of houses and you get anything from an antique farmhouse to a 20's Tudor to new construction. Croton residents have a lovely beach on the Croton River (Silver Lake), and in the summer there are regular concerts and movies at Senasqua park on the Hudson (the park is residents only, but the events are open to all). Croton Point Park is great, and the Croton Landing Park is really amazing. The nearby towns offer a huge numbr of parks and preserves, notably
Teatown Lake Reservation which also has excelelnt nature classes and camps for kids.
We have friends in Croton whose kids get special services and they've been happy so far, although it is evidently getting much harder to get the needed sevices as budgets get tighter. How "good" a school system is depends on how you meansure that--but I think that Croton schools are certainly very good by any measurement.
Croton is low on commercial offerings, but there is a good coffee house, excellent gourmet food store, a handful of good restaurants, and enough big box stores. You can get more big box stores about 10 minutes north in Cortlandt on Route 6 or in Ossining or Mt Kisco, and there are a lot more interesting restaurants, stores, galleries, etc in Mt Kisco, Peekskill, and other nearby towns. A lot of our Croton friends go to downtown Yorktown Heights (about 15 minutes) for food shopping.
Croton is pretty diverse socio-economically. The town has a history of having a large working-class community and a large community of artists, academics, and creative professionals. The local elections have gotten really nasty lately. The mayor won by 51% and there is still a lot of animosity and bad feelings.