AbstractA gravimetric method for the determination of surface excess isotherms of compressed gases on solid adsorbents is described. Buoyancy corrections are minimized by using a symmetric‐beam microbalance and by compensating the volume of the adsorbent. — Isotherms of argon and methane onto Graphon (a graphitized carbon black) are determined up to 150 bar at −20, 0, 25, and 50°C, corresponding to bulk densities up to the critical density for methane, and more than half the critical density for argon. Surface excess isotherms exhibit a maximum at about 0.4 to 0.5 of the critical density. The range of applicability of simple isotherm equations for higher gas pressures is discussed b