Recent studies point to an exotic spin-triplet valley-singlet (STVS) superconducting phase in certain two-valley electron liquids, including rhombohedral trilayer graphene, Bernal bilayer graphene and ZrNCl, which nevertheless admits only trivial topology. Here, we predict that upon twisting two layers of STVS superconductors, a chiral $$f\pm {{{{{{{\rm{i}}}}}}}}{f}^{{\prime} }$$ f ± i f ′ -wave superconducting phase emerges near the ‘maximal’ twist angle of 30∘ where the system becomes an extrinsic quasi-crystal with 12-fold tiling. The resulting composite hosts an odd number of chiral Majorana edge modes and a single non-Abelian Majorana zero mode (MZM) in the vortex core. Through detailed symmetry analysis and microscopic modelling, we demonstrate that the non-Abelian topological superconductivity (TSC) forms robustly near the maximal twist when the isolated Fermi pockets coalesce into a single connected Fermi surface in the moiré Brillouin zone. Our results establish the large-twist-angle engineering, with distinct underlying moiré physics from magic-angle graphene, as a viable route toward non-Abelian TSC.

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