Here, we present investigation of the influence of different gases (carbon dioxide, ammonia, and iodine vapor) on the sensory properties of graphene and single-wall carbon nanotube films. The gas molecules are adsorbed by carbon films (graphene or nanotubes) and change the film’s electrical resistance. In the course of this work, the setup for studying the electrophysical properties of carbon nanomaterials has been designed and constructed in the lab. With this home-made equipment, we have demonstrated a high efficiency of graphene and nanotubes as adsorbents of different gases and a possibility to use these materials as gas sensors. We have also performed a chemical modification of graphene and carbon nanotubes by attaching the nanoparticles of calcium carbonate () to improve the sensitivity and selectivity of sensors.