The combination of quantum sensing with quantum computing to provide an enhancement over conventional quantum sensing has recently emerged as a promising potential application of quantum computing that could give advantages without needing large-scale or fault-tolerant hardware. In this work, we report an experimental demonstration of a recent theoretical proposal to repurpose Grover's search algorithm to improve the ability to detect signals with unknown frequency within a large detection bandwidth. Our experiments were based on a system comprising a single superconducting qubit coupled to a single superconducting cavity, highlighting the modest hardware requirements for realizing the protocol. We found that Grover-based sensing was able to outperform the natural non-Grover baseline for our experimental platform for detection bandwidths >10 MHz, with an advantage that empirically grew superlinearly with the bandwidth beyond that break-even point. The use of the Grover-based protocol reduced the amount of signal that needed to be sensed to make an accurate detection decision by more than 10× for choices of larger detection bandwidth and higher desired detection accuracy. Our results provide a proof-of-principle validation that Grover-based quantum computational sensing can be realized in near-term hardware and provide a metrological advantage well beyond break-even in spite of the additional protocol complexity.