In this study, composites of HKUST‐1 MOF with nanocellulose, HKUST‐1@NCs, have been prepared and explored for CO2/N2 gas‐separation and dye‐sorption based applications. Our biopolymer‐MOF composites are prepared via a copper ion pre‐seeding method, in which, the HKUST‐1 crystallites are grown in situ on the Cu‐seeded and carboxylate anchored NC fibers for a better interfacial integration between the MOF and the polymer matrices. Static gas sorption studies show the capability of one of our HKUST‐1@NC composites to reach ∼300 % enhancement in the CO2/N2 sorption selectivity compared to the corresponding MOF alone ‐ blank reference sample prepared at similar conditions. The same composite, C100, in the bulk powder form, shows a remarkable IAST sorption selectivity of 298 (CO2/N2) at 298 K and 1 bar for the CO2/N2 (15/85, v/v) gas mixture. The relative position of the C100, in the bound plot visualizations of the CO2/N2 separation trade‐off factors indicate a significant potential. The HKUST‐1@NC composites have also been processed along with a polymeric cellulose acetate (CA) matrix as HKUST‐1@NC@CA films to study them as free‐standing mixed‐matrix membranes. The CO2/N2 sorption selectivity, at 298 K and 1 bar is 600 for one such membrane, C‐120@CA, as bulk sample studied by the static gas sorption. The composite, C120, exhibits a good uptake with an enhancement of 11 % for alizarin and 70 % for Congo red in comparison to the uptakes of the corresponding blank reference HKUST‐1 sample, B120.