We develop a novel bi-harmonic mathcal{N} = 4 superspace formulation of the mathcal{N} = 4 supersymmetric Yang-Mills theory (SYM) in four dimensions. In this approach, the mathcal{N} = 4 SYM superfield constraints are solved in terms of on-shell mathcal{N} = 2 harmonic superfields. Such an approach provides a convenient tool of constructing the manifestly mathcal{N} = 4 supersymmetric invariants and further rewriting them in mathcal{N} = 2 harmonic superspace. In particular, we present mathcal{N} = 4 superfield form of the leading term in the mathcal{N} = 4 SYM effective action which was known previously in mathcal{N} = 2 superspace formulation.