Planar laser-induced fluorescence (PLIF) was applied for the first time in the 20-ft vacuum chamber at the Marshall Space Flight Center to visualize the plume-surface interaction (PSI) of a nitrogen jet seeded with nitric oxide (NO). A Mach 5.3 nozzle was used to simulate the exhaust of a landing spacecraft for two different jet stagnation pressures and one jet stagnation temperature. A flat plate was used to simulate the landing surface, and two different dimensionless altitudes were investigated. The chamber pressure was reduced such that both lunar-relevant environments at 0.01–28 Pa and Martian-relevant environments at ∼600 Pa were investigated. PLIF flow visualization was performed using a pulsed, tunable, ultraviolet laser, which entered the vacuum chamber through a window, and was directed to the test article using remote-controlled mirrors. Fluorescence at ultraviolet wavelengths was imaged using an intensified camera, which was placed inside a pressurized enclosure located inside the vacuum chamber. For the Martian-relevant condition, a Mach disk and stagnation bubble were observed at h/De = 10, whereas a pair of oblique stagnation shocks were observed at h/De = 3. Significantly complex flows, such as different stagnation shock behaviors, were observed for the lunar-relevant conditions based on the h/De and Reynolds number. The results presented here are the first NO-PLIF measurements of the PSI flowfield within rarefied environments. The unique information on jet expansion and plume structure will be useful to aid researchers in validating complex computational simulations and to inform engineering designs of extraterrestrial landing systems.