This paper presents a VCO-based EPR-on-a-chip (EPRoC) sensor for portable, battery-operated electron paramagnetic resonance (EPR) spectrometers. The proposed chip contains an array of 14 injection-locked VCOs as the sensing element for an improved sensitive volume and phase noise performance. By cointegrating a high-bandwidth PLL, the presented design allows for continuous-wave and rapid-scan EPR experiments with a minimum number of external components. The active loop filter introduces an assisted replica charge pump that mitigates the slewing requirements on the loop-filter amplifier. The measured spin sensitivity of 2×10 9 spins/Hz−−−√ together with the large active volume of 210 nl lead to an 8-fold improvement in concentration sensitivity compared to the state-of-the-art in EPRoC detectors.