Approximately 600 to 500 million years ago, a major evolutionary radiation called the “Cambrian Explosion” gave rise to nearly all of the major animal phyla known today. This radiation is recorded by various fossil lagerstätten, such as the Burgess Shale in Canada, where soft-bodied animals are preserved in exquisite detail. Many Cambrian fossils are enigmatic forms that are morphologically dissimilar to their modern descendants, but which still provide valuable information when interpreted as stem-group taxa because they record the actual progression of evolution and give insight into the order of character acquisitions and homologies between living taxa. One such group of fossils is the anomalocaridids, large presumed predators that have had a complicated history of description. Their body has a trunk with a series of lateral lobes and associated gills, and a cephalic region with a pair of large frontal appendages, a circular mouth apparatus, stalked eyes and a cephalic carapace. Originally, two taxa were described from the Burgess Shale, Anomalocaris and Laggania, however data presented herein suggests that the diversity of the anomalocaridids was much higher. Newly collected fossil material revealed that a third Burgess Shale anomalocaridid, Hurdia, is known from whole-body specimens and study of its morphology has helped to clarify the morphology and systematics of the whole group. Hurdia is distinguished by having mouthparts with extra rows of teeth, a unique frontal appendage, and a large frontal carapace. Two species, Hurdia victoria and Hurdia triangulata were distinguished based on morphometric shape analysis of the frontal carapace. A phylogenetic analysis placed the anomalocaridids in the stem lineage to the euarthropods, and examination of Hurdia’s well-preserved gills confirm the homology of this structure with the outer branches of limbs in upper stem-group arthropods. This homology supports the theory that the Cambrian biramous limb formed by the fusion of a uniramous walking limb with a lateral lobe structure bearing gill blades. In this context, new evidence is present on the closely allied taxon Opabinia, suggesting that it had lobopod walking limbs and a lateral lobe structure with attached Hurdia-like gills. The diversity of the anomalocaridids at the Burgess Shale is further increased by two additional taxa known from isolated frontal appendages. Amplectobelua stephenensis is the first occurrence of this genus outside of the Chengjiang fauna in China, but Caryosyntrips serratus is an appendage unique to the Burgess Shale. To gain a better understanding of global distribution, a possible anomalocaridid is also described from the Sirius Passet biota in North Greenland. Tamisiocaris borealis is known from a single appendage, which is similar to Anomalocaris but unsegmented, suggesting this taxon belongs to the arthropod stem-lineage, perhaps in the anomalocaridid clade. Thus, the anomalocaridids are a widely distributed and highly diverse group of large Cambrian presumed predators, which provide important information relevant to the evolution of the arthropods.