We study the largest-angle twisted homo-bilayer (LA-THB) systems, hosting Moiréless quasicrystal (QC) structure. We propose to use these materials to generate high-angular-momentum (HAM) topological superconductivities (TSCs) protected by their QC symmetries absent on conventional crystalline materials. This proposal is based on our universal Ginzburg-Landau theory based analysis which yields the general conclusion that, when each Dn-symmetric (n is even) monolayer hosts SC with pairing angular momentum l ≤ n 2 , the interlayer Josephson coupling will induce SC with pairing angular momentum L = l or L = n − l in the LA-THB, determined by microscopic details. The latter one is just the HAM TSC if l > 0. Based on our revised perturbational-band theory, we develop general microscopic framework to study the QC LA-THBs involving electronelectron interactions, adopting which we study three examples, i.e. the 30 • -twisted bilayer graphene, the 30 • -twisted bilayer BC3, and the 45 • -twisted bilayer cuprates. The g + ig-h + ih-and d + id-TSCs with HAM L = 4, 5 and 2 can emerge in certain doping regimes in these systems, respectively.