Abstract: In the heterogeneous photocatalytic degradation of environmental contaminants the recovery, reuse of employed nanocatalyst was crucial and it is essentially required for the scale up applications. Besides, designing a magnetic material with heterojunction that can effectively oxidize the toxic organic contaminants to non-toxic substance under different reaction conditions including direct solar light irradiation remains a challenge. Considering the above facts, herein, we tailored heterojunction between the magnetic materials and non-magnetic materials with ultra-small Ni nanoparticles modified NiFe2O4/TiO2 nanostructures (Ni@NiFe2O4/TiO2 magnetic nanocomposites) through a simple sonochemical route. The Raman phonons at similar to 540 cm(-1) consistent to nickel metal nanoparticles and the spinel ferrites crystal structure confirmed the formation of Ni@NiFe2O4/TiO2 magnetic nanocomposites. The reduced optical bandgap of the resulting nanocomposites indicated the effective absorption of direct solar light irradiation when compared to the bare TiO2. Thus in-turn, enhanced the photocatalytic efficiency of simazine degradation in the presence of Ni@NiFe2O4/TiO2 magnetic nanocomposites (k= 11.0 x 10(-4) s(-1)) and augmented the activation of peroxymonosulphate (PMS) in the presence of Ni@NiFe2O4/TiO2 magnetic nanocomposites (k= 32.5 x 10(-4) s(-1)). Ni@NiFe2O4/TiO2 +PMS exhibited 3 folds enhanced efficiency in the presence of sunlight. The as-prepared NiFe2O4/TiO2 magnetic nanocatalysts were more stable and the efficiency of simazine oxidation was approximately same for the continuous five cycles at the optimized experimental conditions. The Ni@NiFe2O4/TiO2 magnetic nanocomposites preparation and the activation of PMS may promise the applications in an efficient wastewater treatment.