Andrew, try this approach. It uses IsApproved rather than the IsLockedOut. If your implementation does not already use IsAproved, this would be a good solution.
MembershipUser muUser = Membership.GetUser(strUsernameToActOn);
muUser.IsApproved = false;
Membership.UpdateUser(muUser);
This is not exactly locking the user. Technically this call is taking approved status from the user and leaving them unable to log-in.