In this study, polysulfone/polyvinylpyrrolidone (PSf/PVP, 20 wt%/5 wt%)-based ultrafiltration (UF) membranes reinforced with different ratios (0.5 and 1 wt%) of cellulose nanocrystals (CNCs) and cellulose nanofibres (CNFs) were prepared by the phase inversion method. The effect of CNC, CNF, and CNC-CNF reinforcement on the morphology, roughness, crystallinity, porosity, average pore size, mechanical properties, and filtration performance of PSf/PVP-based membrane was investigated. Distilled water and surface water (lake water) fluxes of the membranes were determined at 3 bar using a dead-end filtration system. The distilled water flux of the fouled–hydraulic cleaned membranes was determined, and scanning electron microscopy (SEM) images of the fouled–cleaned membranes were examined. The flux recovery ratio (FRR) and fouling parameters were calculated to examine the fouling behaviour of the membranes. The mechanical properties of the membranes were modelled by the Mori–Tanaka, finite element, Voigt–Reuss, self-consistent scheme, and Halpin–Tsai methods using Digimat and/or analytically. In addition, the von Mises equivalent stress distributions of the nanocomposites were presented. Among the investigated membranes, PSf/PVP/CNC-0.5 had the highest distilled water flux (475.5 ± 17.77 L/m2.h), PSf/PVP/CNF-1 exhibited the stiffest behaviour with an elasticity modulus of 70.63 ± 3.15 MPa, and PSf/PVP/CNC-1 had the best organic matter removal efficiency. The finite element was the most successful modelling method for estimating the mechanical properties of nanocellulose-reinforced flat sheet membranes.