Polyvinylidene fluoride (PVDF) membrane was improved using TiO2 nanoparticles and nanocellulose for membrane distillation crystallization in this work. Besides the addition of TiO2 nanoparticles and nanocellulose, PVDF membrane was post-modified with octadecyltrichlorosilane after phase inversion using a dual coagulation bath. The addition of hydrophilic TiO2 nanoparticles and nanocellulose reduced membrane hydrophobicity, but the dispersed TiO2 nanoparticles assisted silane modification to improve surface hydrophobicity. Besides reducing the agglomeration of TiO2 nanoparticles, nanocellulose induced the formation of larger pore size and higher porosity as proven in SEM images and gravimetric measurement, respectively. The abundant moieties of nanocellulose accelerated the exchange between solvent and non-solvent during phase inversion for the formation of large pore size and porosity, but membrane thickness increased due to the thickening effects. The modified membrane showed higher water permeate flux in membrane distillation with salt rejection greater than 97%. Severe fouling in membrane distillation crystallization was not observed.