Mn+1AXn (MAX) phases have attracted significant attention due to their structural diversity and potential applications. Designing MAX phases with single-atom-thick A layers featuring 4d/5d-orbital electronic elements is interesting work. Here, we present a comprehensive report on noble metal-based M2(A1-xA′x)C (M = V, Ti, Nb; A = Al, Sn, In, Ga, Ge; A′ = Ru, Rh, Pd, Ir, Pt, Au and combinations thereof; 0 < x ≤ 0.4) phases featuring A sublayers of 4d/5d-orbital electronic elements through an A-site alloying strategy. The chemical composition of MAX phases can be adjusted by selecting different M- and A-site elements, with morphology tailored by distinct C sources. Furthermore, the V2(Sn0.8Pt0.2)C (15.7 wt % Pt) catalyst showed better performance for hydrogen evolution reaction compared to the commercial Pt/C (20 wt % Pt) electrode. This study highlights the prospects of A-site alloying for the design of novel MAX phases with unique properties and promising applications in electrocatalysis and beyond.