Isolated, well‐preserved silicified sclerites of an unusually diverse Silurian paleoloricate assemblage from Gotland preserve morphological features that are important in interpreting palaeobiology. The typically granular dorsal ornament is comparable with Recent chitons, and is hence possibly linked functionally with sensory aesthetes. Ventral structures particularly in thickened shells indicate major muscle attachment sites sub‐apically or, equivalently, beneath the rim of the apical area, and also marginally. In early chitons such as Cambrian Matthevia, deep ventral cavities represent comparable sub‐apical sites. Three Gotland genera with an unusual, holoperipheral shell growth style apparently represent plated aplacophorans (cf. Acaenoplax), which coexisted with paleoloricate chitons in shallow inshore carbonate shelf environments. Sclerite features of all the Gotland genera are discussed together since they share most characteristics. The new family Heloplacidae includes those genera and Acaenoplax, which in a preliminary cladistic analysis form a sister group to other Lower Palaeozoic paleoloricates. Multiplated skeletons in paleoloricates and this group of aplacophorans represent parallel evolution of dorsal armour, which in chitons resulted in overlapping, articulating sclerites. The diversity of the mid‐Silurian Gotland assemblage is examined against early evolutionary diversification of polyplacophorans, aplacophorans, and in relation to the overall record of Palaeozoic paleoloricate and neoloricate chitons. Peaks in diversity in early Ordovician, mid‐Silurian and early Carboniferous times correspond to periods with widespread development of low latitude carbonate shelves. Neoloricates, apparently with an additional shell layer that contributed articulatory plates, appeared in the Devonian from where the fossil record remains poorly known.