In this paper, a time-domain magnetorelaxometry biosensing scheme is presented using giant magnetoresistive (GMR) sensors to measure the fast relaxation response of superparamagnetic magnetic nanoparticles (MNPs) in a pulsed magnetic field. The system consists of an 8 × 10 GMR sensor array, a Helmholtz coil, an electromagnet driver, and an integrator-based analog front-end needed to capture the fast relaxation dynamics of MNPs. A custom designed electromagnet driver and Helmholtz coil improve the switch-off speed to >5 Oe/μs, limiting the dead zone time to <10 μs, and thus enables the system to monitor fast relaxation processes of 30 nm MNPs. A magnetic correlated double sampling technique is proposed to reduce sensor-to-sensor variation by 99.98% while also reducing temperature drift, circuit offset, and nonlinearity below the noise level. An optimum integration time is calculated and experimentally verified to maximize the SNR. Experiments with dried MNPs have shown successful relaxation detection, and immunoassay experiments have demonstrated their binding kinetics.