The zodiacal dust complex, a population of dust and small particles that pervades the solar system, provides important insight into the formation and dynamics of planets, comets, asteroids, and other bodies. We present a new set of data obtained from direct measurements of momentum transfer to a spacecraft from individual particle impacts. This technique is made possible by the extreme precision of the instruments flown on the LISA Pathfinder spacecraft, a technology demonstrator for a future space-based gravitational wave observatory. Pathfinder employed a technique known as drag-free control that achieved rejection of external disturbances, including particle impacts, using a micropropulsion system. Using a simple model of the impacts and knowledge of the control system, we show that it is possible to detect impacts and measure properties such as the transferred momentum, direction of travel, and location of impact on the spacecraft. In this paper, we present the results of a systematic search for impacts during 4348 hr of Pathfinder data. We report a total of 54 candidates with transferred momenta ranging from 0.2 to 230 μNs. We furthermore make a comparison of these candidates with models of micrometeoroid populations in the inner solar system, including those resulting from Jupiter-family comets (JFCs), Oort Cloud comets, Halley-type comets, and asteroids. We find that our measured population is consistent with a population dominated by JFCs, with some evidence for a smaller contribution from Halley-type comets, in agreement with consensus models of the zodiacal dust complex in the momentum range sampled by LISA Pathfinder.