We report a versatile synthetic process based on rapid heating and cooling chemical vapor deposition for the growth of carbon nanotube (CNT)-graphene hybrid materials where the thickness of graphene and density of CNTs are properly controlled. Graphene films are demonstrated as an efficient barrier layer for preventing poisoning of iron nanoparticles, which catalyze the growth of CNTs on copper substrates. Based on this method, the opto-electronic and field emission properties of graphene integrated with CNTs can be remarkably tailored. A graphene film exhibits a sheet resistance of 2.15 kΩ sq(-1) with a transmittance of 85.6% (at 550 nm), while a CNT-graphene hybrid film shows an improved sheet resistance of 420 Ω sq(-1) with an optical transmittance of 72.9%. Moreover, CNT-graphene films are demonstrated as effective electron field emitters with low turn-on and threshold electric fields of 2.9 and 3.3 V μm(-1), respectively. The development of CNT-graphene films with a wide range of tunable properties presented in this study shows promising applications in flexible opto-electronic, energy, and sensor devices.