Organic–inorganic nanoparticles, which can improve and modify the mechanical and chemical properties of polymers, have been used as fillers to prepare high-performance hybrid nanocomposite membranes. In this study, we explored whether the incorporation of organic nanofillers (graphene (G), graphene oxide (GO), carbon nanotubes (CNTs), or oxidized carbon nanotubes (CNTOxi)) into polysulfone (PSF) and montmorillonite (MMt)-modified PSF membranes could enhance membrane performance for the removal of heavy metal ions from contaminated solutions. These hybrid membranes were prepared by a phase inversion method using chloroform as the solvent. The surface morphologies of the membranes revealed good dispersibility of the organoclay and carbon nanomaterials in the PSF matrix. The hybrid nanocomposite membranes showed significantly improved thermal stability and mechanical properties as compared to the pristine PSF and PSF/MMt membranes. The adsorption efficiencies of these hybrid adsorptive membranes for Hg(II), Pb(II), Sr(II), Fe(III), Zn(II), Ni(II), Al(III), Co(II), Y(III), and Cr(III) were investigated. The PSF/MMt/CNTOxi and PSF/MMt/GO membranes exhibited the highest adsorption efficiencies. In particular, these adsorptive membranes showed selectivity toward Hg(II), and the Hg(II) extraction percentage was maximized at pH 2. The maximum Hg(II) adsorption capacities of PSF/MMt/CNTOxi and PSF/MMt/GO were 151.36 and 144.89 mg/g, respectively, and the adsorption isotherm was in approval with the Langmuir model. These hybrid nanocomposites can be used in water purification application.