We demonstrate a versatile single‐laser platform for single‐beam dual‐color two‐photon spectroscopy that combines a short‐pulse laser source with a tunable broadband wavelength converter based on a highly nonlinear photonic‐crystal fiber (PCF). We show that the short‐pulse PCF output can be tailored, via dispersion and nonlinearity management, to deliver a broadband optical driver whose spectral structure is ideally suited for a single‐beam two‐photon absorption (2PA) spectroscopy of the next‐generation genetically encodable fluorescent‐protein (FP) sensors of pH and redox‐responsive contrast agents. As a promising spectroscopic resource for redox biology, the short‐pulse PCF output can be finely sculpted to alternately drive an FP system via a one of its two 2PA‐allowed quantum pathways, yielding a high‐contrast fluorescence readout for a highly sensitive detection of redox reactions and signaling, pH sensing, and oxidative‐stress diagnosis. We demonstrate a versatile single‐laser platform for single‐beam dual‐color two‐photon spectroscopy that combines a short‐pulse laser source with a tunable broadband wavelength converter based on a highly nonlinear photonic‐crystal fiber. This approach suggests a promising spectroscopic resource for a highly sensitive detection of redox reactions and signaling, pH sensing, and oxidative‐stress diagnosis.