In Bi2Te2Se the defect chemistry involves native defects that compete such that they can either exchange dominance or else significantly compensate each other. Here we show how the net carrier concentration, n − p, which depends on the relative amounts of these defects and is readily obtained from Hall data, can be used as a fundamental materials parameter to describe the varied behavior of the thermoelectric properties as a function of compensation. We report the effects of tuning this parameter over multiple orders of magnitude by hole-doping the n-type material Bi2Te2Se0.995, which is already significantly compensated because of its Se deficiency. Crystals with different levels of hole doping were achieved by two separate approaches, namely by selecting pieces from different locations in an undoped crystal in which a systematic carrier concentration gradient had been induced by its growth conditions, and alternatively by doping with Sn for Bi. The thermoelectric power factors for Bi2−xSnxTe2Se0.995 for x = 0, 0.002, 0.005, 0.010, and 0.040 are reported, and the dependence of the transport properties on the extent of compensation is discussed.