Information about the elemental composition of a planetary surface can be determined using nuclear instrumentation such as gamma-ray and neutron spectrometers (GRNS). High-energy Galactic Cosmic Rays (GCRs) resulting from cosmic super novae isotropically bombard the surfaces of planetary bodies in space. When GCRs interact with a body’s surface, they can liberate neutrons in a process called spallation, resulting in neutrons and gamma rays being emitted from the planet’s surface; how GCRs and source particles (i.e. active neutron generators) interact with nearby nuclei defines the nuclear environment. In this work I describe the development of nuclear detection systems and techniques for future orbital and landed missions, as well as the implications of nuclear environments on a non-silicate (icy) planetary body. This work aids in the development of future NASA and international missions by presenting many of the capabilities and limitations of nuclear detection systems for a variety of planetary bodies (Earth, the Moon, metallic asteroids, icy moons). From bench top experiments to theoretical simulations, from geochemical hypotheses to instrument calibrations—nuclear planetary science is a challenging and rapidly expanding multidisciplinary field. In this work (1) I describe ground-truth verification of the neutron die-away method using a new type of elpasolite (Cs2YLiCl6:Ce) scintillator, (2) I explore the potential use of temporal neutron measurements on the surface of Titan through Monte-Carlo simulation models, and (3) I report on the experimental spatial efficiency and calibration details of the miniature neutron spectrometer (Mini-NS) on board the NASA LunaH-Map mission. This work presents a subset of planetary nuclear science and its many challenges in humanity's ongoing effort to explore strange new worlds.