No, object initializer is the only place where assignment syntax like that can be used. If you need to assign multiple fields at once from many different places in code without duplication, you could define a method that encapsulates all the assignments for you:
void SetNameAndGender(string f, string l, bool isMale) {
FirstName = f;
LastName = l;
IsMale = isMale;
}
Unfortunately, it does not let you set an arbitrary group of properties, like the VB syntax that you show.