We report the application of molecular tagging velocimetry (MTV) toward two-component velocimetry as demonstrated in an underexpanded free jet flowfield. Two variants of the MTV technique are presented: 1) electronic excitation of seeded nitric oxide (NO) with gated fluorescence imaging (fluorescence lifetime) and 2) photodissociation of seeded ${\mathrm{NO}}_2$ followed by NO fluorescence imaging ( ${\mathrm{NO}}_2$ photodissociation). The seeded NO fluorescence lifetime technique is advantageous in low-quenching, high-velocity flowfields, while the photodissociation technique is useful in high-quenching environments, and either high- or low-velocity flowfields due to long lifetime of the NO photoproduct. Both techniques are viable for single-shot measurements, with determined root mean squared results for streamwise and radial velocities of $\sim 5\%$ . This study represents the first known application of MTV utilizing either the fluorescence lifetime or the photodissociation technique toward two-component velocity mapping in a gaseous flowfield. Methods for increasing the spatial resolution to be comparable to particle-based tracking techniques are discussed.