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This book reports on the full-stack experimental search (from inception to discovery) of the first observation of neutrino-induced fission. Over fifty years ago, physicists predicted that neutrinos, such as those from supernova or nuclear reactors, could fission heavy nuclei. This "new way to split the atom" could serve as an exciting new way to observe low-energy neutrinos and would also play an important role in the creation of heavy nuclei in neutrino-rich astrophysical environments-for instance, in the R-process for nucleosynthesis. The challenge in detecting this interaction and thus confirming its existence was twofold: the neutrino interacts only rarely; and the targets of interest must be fissionable, and therefore already produce large radioactive backgrounds. This landmark thesis describes the inception, design, construction, and operation of the first measurement of neutrino-induced fission and the presentation of the first exciting results from the work. It is the first measurement of neutrino-induced fission and the first measurement of a neutrino cross-section on an unstable nucleus. The work is an open door for new experiments designed to search for new "NuFission" interactions and find new applications for this new approach to neutrino detection.