We report the identification of 89 new systems containing ultracool dwarf companions to main-sequence stars and white dwarfs, using the citizen science project Backyard Worlds: Planet 9 and cross-reference between Gaia and CatWISE2020. 32 of these companions and 33 host stars were followed up with spectroscopic observations, with companion spectral types ranging from M7-T9 and host spectral types ranging from G2-M9. These systems exhibit diverse characteristics, from young to old ages, blue to very red spectral morphologies, potential membership to known young moving groups, and evidence of spectral binarity in nine companions. 20 of the host stars in our sample show evidence for higher-order multiplicity, with an additional 11 host stars being resolved binaries themselves. We compare this sample's characteristics with those of the known stellar binary and exoplanet populations, and find our sample begins to fill in the gap between directly imaged exoplanets and stellar binaries on mass ratio-binding energy plots. With this study, we increase the population of ultracool dwarf companions to FGK stars by ~42%, and more than triple the known population of ultracool dwarf companions with separations larger than 1000AU, providing excellent targets for future atmospheric retrievals.