Multifunctional　integration　of　optoelectronic　devices　within　a　single　photodiode　is　in　high　demand　for　next-generation　on-chip　multifunctional　integration　and　Internet　of　Things　applications.　Owing　to　the　rapidity　of　nucleation-crystallization　that　is　associated　with　the　solution　method,　large　trap　state　densities　(N-t),　and　consequently,　severe　dark　current　densities,　as　well　as　recombination　losses　are　generally　induced,　which　are　detrimental　to　the　detectivity　(D*)　of　organic　photodetectors　(OPDs)　and　to　the　open-circuit　voltage　(V-OC)　of　organic　photovoltaics　(OPVs).　Herein,　a　versatile　p-i-n　heterojunction　organic　photodiode　with　optimized　vertical　phase　distribution　and　rational　solid-state　packing　is　fabricated　via　a　layer-by-layer　(LBL)　deposition　procedure　entailing　the　introduction　of　a　rylene-fullerene　hybrid　as　a　morphological　modulator.　This　precisely　controlled　photodiode　displayed　suppressed　N-t　(2.5　x　10(16)　cm(-3)),　low-lying　Urbach　energy　E-u　(23.2　meV),　as　well　as　synergistically　reduced　series　resistance,　dark　current,　and　sub-bandgap　radiative/non-radiative　recombination　losses.　Consequently,　this　ternary-pseudo-bilayer-type　photodiode　exhibits　excellent　dual-function　performance　with　an　outstanding　D*　of　9.48　x　10(11)　Jones　in　self-powered　OPD　mode　and　a　surprisingly　suppressed　energy　loss　of　0.538　eV　in　OPV　mode.　This　study　provides　important　insights　into　the　mechanism　and　effects　of　trap　density　and　energy　disorder　suppression　in　solution-processed　multifunctional　integrated　photoelectric　conversion　diodes.