I do not think there is either function (nor indeed a non-brute force algorithm), though presumably asymptotically most matrices are invertible, so building matrices and testing invertibility would not be abysmal overkill.
Thus a very basic version (here for 0/1) is to take sets of possible rows (as combinations of different vectors) first (which saves on a factor of $n!$) before testing invertibility:
gap> n:=5;
gap> zeroone:=Combinations(Tuples([0,1],n),n);;Length(zeroone);
201376
gap> zeroone:=Filtered(zeroone,x->not IsZero(DeterminantMat(x)));;Length(zeroone);
104286
Then all matrices are obtained by permuting rows:
gap> sym:=SymmetricGroup(n);;
gap> all:=Concatenation(List(zeroone,x->Orbit(sym,x,Permuted)));;
which will get all 12514320 matrices.