Glacial strata are excellent stratigraphic markers in Paleozoic basins worldwide. The eastern Parnaíba Basin in northern Brazil is a highly favorable setting for studying episodes related to the Ordovician-Silurian glaciation. Previous studies in this region led to the recognition of unequivocally glaciogenic sediments associated with pre- and postglacial deposits, favoring the understanding of lower Paleozoic events that occurred in West Gondwana. Outcrop-based facies and stratigraphic analyses of the ~170 m-thick siliciclastic succession of the Serra Grande Group indicate fluvial, glacial, and coastal depositional systems. Seventeen sedimentary facies are grouped into seven facies associations (FAs): FA1, interpreted as intermediary sheet braided plain deposits that consist of tabular cross-bedded coarse-grained sandstones and conglomerates; FA2-FA4, which correspond to subaqueous glacial deposits comprising massive to stratified diamictites, cross-laminated sandstones, diamictites and organic matter-rich black shales with dumpstone and dropstone structures; FA5-FA6, constituting organic matter-rich black shales, fine- to medium-grained sandstones with sigmoidal cross-bedding and occurrences of the ichnotaxon Arthrophycus interpreted as delta front deposits; and FA7, composed of medium- to coarse-grained pebbly sandstones interpreted as channelized braided plain deposits. This interpretation partially confirms the previous paleoenvironmental interpretation discounting the presence of subaerial alluvial fan and outwash plain deposits for this unit. The sequence stratigraphy of the Serra Grande Group is refined mainly using the coherent interpretation of the key surfaces and comparing the systems tracts with the global sea-level curve, providing a more robust third-order sequential evolutionary model that includes three depositional sequences. The Middle Ordovician sheet braided deposits are the lowstand sediments of Sequence 1 truncated by an extensive unconformity that possibly removed the transgressive and highstand strata. This unconformity generated by glacial dynamics represents 23 Myr during the Late Ordovician to early Silurian. The second sequence started with the advance of ice sheets in marginal areas of the basin, causing the deposition of ablation diamicton during the lowstand. The postglacial transgression is marked by ice-rafted debris from icebergs deposited onto organic matter-rich mud in the shoreface-offshore zone. The maximum flooding during the middle to late Silurian was succeeded by the highstand phase marked by the progradation of deltaic deposits. Biological activity is marked by the presence of polychaetes that reworked the marine seafloor. The Early Devonian featured extensive sea-level fall and renewed continental drainage with the formation of a braided plain marking a lowstand phase of Sequence 3. These new interpretations allow the global correlation of the Serra Grande Group and provide an improved understanding of the role of ice sheets and postglacial transgressions that affected West Gondwana during the Ordovician-Silurian periods.