We study the higher Chow groups CH^2(X,1) and CH^3(X,2) of smooth, projective algebraic surfaces over a field of char 0. We develop a theoretical framework to study them by using so-called higher normal functions and higher infinitesimal invariants when the cycles are supported on normal crossing divisors. Then we investigate their structure on hypersurfaces in projective 3-space. This leads to vanishing or decomposbility results. On the other hand we find examples of these groups in degrees 4 and 5 where the result is a highly indecomposably (hence big) abelian group. Part of the examples are due to Alberto Collino.