During the latest Neoproterozoic to Mid-Cambrian time (580–505 Ma ago), the Earth underwent significant changes in palaeogeography that included rifting of a possible supercontinent and the near simultaneous formation of a second, slightly smaller supercontinent. It is against this tectonic backdrop that the Cambrian radiation occurred. Although the general tectonic setting during this interval is fairly well constrained, models of the exact palaeogeography are controversial because of the lack of reliable palaeomagnetic data from some of the continental blocks. Palaeogeographical models based on palaeomagnetic data range from a high-latitude configuration for most continents, to a low-latitude configuration for most continents, or to rapid oscillations in continental configurations triggered by inertial changes within the planet. Palaeobiogeographical data can also be used to help constrain palaeogeographical models. To this end we use vicariance patterns in olenellid trilobites to determine their compatibility with three end-member palaeogeographical models derived from palaeomagnetic data for the Neoproterozoic and early Cambrian. The most congruent palaeogeographical model with respect to the palaeobiogeographical data described herein is the high-latitude configuration for most continents. Those palaeomagnetic models that predict inertial interchange true polar wander or multiple episodes of true polar wander differ significantly from the results from palaeobiogeography. The low-latitude palaeogeographical models also differ from the results from palaeobiogeography, but this may partly arise because of a lack of palaeomagnetic and palaeobiogeographical data from many parts of present-day South America and Africa.