A modular system is described to measure thermally stimulated current (TSC) in irradiated metal-oxide-semiconductor (MOS) capacitors. Custom capacitor mounting allows accurate and convenient measurement of TSC with less than ∼0.1 pA error at temperatures up to ∼300 °C. These measurements are used to estimate the densities and energy levels of defects in the 1SiO2 layer of irradiated MOS capacitors with 45, 98, and 350 nm oxides. For capacitors irradiated under positive bias, TSC measurements provide accurate estimates of radiation-induced trapped-positive-charge density only if performed under negative bias. It is shown that space-charge effects and capacitance changes during TSC measurement can lead to incorrect estimates of the radiation-induced trapped-charge density. We demonstrate that, for n-substrate capacitors, these effects can be minimized if the bias applied during TSC measurement is more negative than the inversion-point voltage on a post-irradiation capacitance-voltage (C-V) curve. This improves prior practice in the literature. Improved estimates are provided for trapped hole energies in SiO2. Further, TSC measurements under proper bias conditions can be combined with conventional high-frequency C-V measurements to estimate hole- and electron-trap densities near the Si/SiO2 interface of irradiated MOS capacitors. To our knowledge, no other method can be used to quantitatively separate the effects of positive and negative oxide-trap charge on the radiation response of MOS devices. Finally, we show that irradiation with ∼10 keV x rays or ∼1.25 MeV Co-60 gamma rays leads to similar trapped-hole densities and energies in MOS capacitors with 350 nm nonradiation-hardened oxides.