Thousand Oaks is definitely family friendly and the public school system is good according to my cousin whose kids go went to elementry, middle and high school. In fact, her daughter just got accepted to Berekely to study sociology. However, Santa Monica is closer to LA and more central to the large business centers. Some things to think about (if you don't have already or need to) are emplyment and the location of emplyment. If you are comfortable with commuting, if needed (Traffic can be grewling in LA and Ventura), high paced or lower paced neighborhoods, any particular community needs, family close/ far, climate preferences, just throwing ideas out there.
Personally, I am an advocate of private schools and I know that both Thousand Oaks and Santa Monica have a few to pick from.
If I were you I would get pre-approved by a lender (if you are thinking of buying), know for sure what my price range is I am looking for, and start comparing Santa Monica with Thousand Oaks with the based on what my needs are and what appeals to me best. Agents can help you answer questions about areas in details, and most are more than willing to spend time showing you around thier local service area, Especially if you are pre-approved!
Hope this helps!
James and Tania Kirchner