Cantanhez National Park in southern Guinea-Bissau is a mosaic of forest, mangrove, savanna, and agricultural fields, with a high prevalence of oil-palm trees (Elaeis guineensis). It hosts many different animal species, including the chimpanzee (Pan troglodytes verus). Very little is known about the ecology of chimpanzees inhabiting this area. The main aims of this study were to evaluate chimpanzee nesting behavior, define trends of habitat use, and estimate chimpanzee density in four separate forests by applying the marked nest counts methodology. From the 287 new nests counted, 92% were built in oil-palm trees with a significantly higher frequency of nests in the forest edge than in forest cores. Differences in nest detection rates were observed in the four monitored forests, with two forests being more important for chimpanzee's nesting demands. The number of nests documented in the forests seemed to be correlated with the frequency of other signs of chimpanzee activity. Although chimpanzees selected nests on the forest edge, they were most frequently observed in forest core areas. Constraints associated with estimating chimpanzee density through oil-palm nest counting are discussed.