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In this article, novel nanocomposites of poly(3- or m-aminobenzenesulfonic acid) and TiO2 were synthesized by very simple in-situ polymerization of monomer (m-ABS) by FeCl3.6H2O as an oxidant and TiO2 particles as inorganic phase under solid-state condition. The combination of N-type TiO2 and P-type PABS led to the preparation of two new P–N junction type nanocomposites. The polymer-hybrid solar cells were fabricated using the nanocomposites as FTO/TiO2/NCPABS-TiO2/Al and under simulated solar irradiation demonstrated power conversion efficiencies (PCE, η) about 1%. The other advantages of this work were fewer fabrication costs, ease-of-processing, green synthesis condition, a simple structure of the solar cell (single layer), and the high stability of the resulted cells. The synthesized nanocomposites (NCPABS-TiO2-1 and 2) were characterized by FT-IR, UV–vis, VSM, XRD, CV, TGA, and CHNS analysis. The electrical properties and conductivity of the nanocomposites were shown that are electro-active and semi-conductive. The morphology of the compounds was investigated by scanning electron microscopy (SEM) and transmission electron microscopy (TEM) that revealed core–shell and nanosheet morphologies, respectively. Also, the effect of core–shell and nanosheet morphology, the presence of -SO3H group, and TiO2 enhancer phase as a separate hole transition layer in solar cell and as an inorganic phase in nanocomposite matrix (active layer) on the power conversion efficiency of hybrid solar cells was investigated. Indeed, it is shown even a small amount of magnetic (nano)material [FeCl2, FeCl3, and/or high spin Fe (ii, iii) complexes] can increase the efficiency of the cell due to conversion of photogenerated state from spin singlet to triplet. [ABSTRACT FROM AUTHOR]