This paper presents a study on control of nanoparticles dispersion in the hard and soft segments of a polyurethane (PU) membrane, via adjusting surface groups of the nanoparticles. The dispersion control allows for tailoring physical and transport properties of the membrane. PU-based mixed-matrix membranes (MMMs) embedded with cyanuric chloride and its derivatives, melamine, and 2,4,6-trihydazino-1,3,5-triazine (THDT) nanoparticles, are prepared. The MMMs are characterized using FTIR, XRD, TGA, DSC, and SEM analyses, and tensile strength tests. Peak assignment of the bonded carbonyl, crystallinity change, mechanical properties of the membranes, possible hydrogen-bonding of the PU backbone and the nanoparticles, and permeation tests indicate that cyanuric chloride nanoparticles are dispersed in the hard segments, whereas melamine and the THDT nanoparticles are distributed in the soft domains. As the cyanuric chloride nanoparticle concentration of the MMMs increases, the gas permeabilities and O-2/N-2, CO2/CH4 and CO2/N-2 selectivities of the membranes increase. In the case of THDT and melamine, as the filler loading increases, the permeabilities of the gases decrease, whereas O-2/N-2, CO2/CH4 and CO2/N-2 selectivities increase. A 10 wt% incorporation of THDT into the PU increases CO2/N-2 and CO2/CH4 selectivities by 92% and 75%, respectively. These results point to the potential of cyanuric chloride nanoparticles for simultaneous improvement of gas permeability and selectivity, and the potential of melamine and THDT nanoparticles for preparation of highly selective nanocomposite membranes for CO2 removal. (C) 2018 Elsevier Ltd. All rights reserved.