Gradient-echo echo-planar imaging (GE EPI) is the most commonly used approach to assess localized blood oxygen level dependent (BOLD) signal changes in real-time. Alternatively, real-time spin-echo single-voxel spectroscopy (SE SVS) has recently been introduced for spatially specific BOLD neurofeedback at 3 T and at 7 T. However, currently it is not known how neurofeedback based on real-time SE SVS compares to real-time GE EPI-based. We therefore compared both methods at high (3 T) and at ultra-high (7 T) magnetic field strengths. We evaluated standard quality measures of both methods for signals originating from the motor cortex, the visual cortex, and for a neurofeedback condition. At 3 T, the data quality of the real-time SE SVS and GE EPI R2* estimates were comparable. At 7 T, the data quality of the real-time GE EPI acquisitions was superior compared to those of the real-time SE SVS. Despite the somehow lower data quality of real-time SE SVS compared to GE EPI at 7 T, SE SVS acquisitions might still be an interesting alternative. Real-time SE SVS allows for a direct and subject-specific T2* estimation and thus for a physiologically more plausible neurofeedback signal.