The carbonization of a newly reported two-dimensional zeolitic imidazolate framework (ZIF-L) with leaf-like morphology was investigated by TG, SEM, XRD and XPS. ZIF-L flakes were thermally stable at up to 200 °C, and completely transformed into an amorphous carbonaceous material after heat treatment in nitrogen at 550 °C. A carbon composite membrane was then prepared by deposition of ZIF-L flakes on a porous alumina support and then direct carbonization of ZIF-L film. During the carbonization, the ZIF-L membrane reorganized into a nanoporous carbon composite membrane composed of ZnO nanoparticles and leaf-like carbon flakes. The resulting nanoporous carbon composite membrane exhibited a narrow micropore size distribution, and it had higher BET surface area than the ZIF-L flakes. Gas separation permeation experiments showed that the carbon composite membrane had a high H2 permeance of 3.5 × 10−6 mol m−2 s−1 Pa−1, and moderate H2/N2 and H2/CO2 ideal selectivities of 6.2 and 4.9, respectively. This work presents a simple and effective method for preparing functional nanoporous carbon composite membranes from ZIFs (or MOFs) for many potential applications.