An environment-friendly insulating gas, perfluoroisobutyronitrile (C4F7N), has been developed recent years. Due to its relatively high liquefaction temperature (around −4.7 °C), buffer gases, such as CO2 and N2, are usually mixed with C4F7N to increase the pressure of the filled insulating medium. During these processes, the insulating gases may be contaminated with micro-water, and the mixture of H2O with C4F7N could produce HF under breakdown voltage condition, which is harmful to the gas insulated electricity transfer equipment. Therefore, removal of H2O and HF in situ from the gas insulated electricity transfer equipment is significant to its operation security. The adsorbents with the ability to remove H2O but without obvious C4F7N/CO2 adsorption capacity are essential to be used in this system. In this work, a series of industrial adsorbents and desiccants were tested for their compatibility with C4F7N/CO2. Pulse adsorption tests were conducted to evaluate the adsorption performance of these adsorbents and desiccants on C4F7N and CO2. The 5A molecular sieve showed high adsorption of C4F7N (22.82 mL/g) and CO2 (43.86 mL/g); F-03 did not show adsorption capacity with C4F7N, however, it adsorbed CO2 (26.2 mL/g) clearly. Some other HF adsorbents, including NaF, CaF2, MgF2, Al(OH)3, and some desiccants including CaCl2, Na2SO4, MgSO4 were tested for their compatibility with C4F7N and CO2, and they showed negligible adsorption capacity on C4F7N and CO2. The results suggested that these adsorbents used in the gas insulated electricity transfer equipment filled with SF6 (mainly 5A and F-03 molecular sieves) are not suitable anymore. The results of this work suggest that it is a good strategy to use a mixture of desiccants and HF adsorbents as new adsorbents in the equipment filled with C4F7N/CO2.