The olive oil industry, recognised for its beneficial products for health and food culture, generates a significant amount of by-products that, if not appropriately managed, can pose considerable environmental challenges. This study examined six olive cakes (OC) from the Trás-os-Montes and Alto Douro regions, collected on different dates and mills: two obtained by pressing (COC), two by centrifugation (TPOC), including one partially pitted and one dehydrated, and two exhausted (EOC), which were subjected to conventional chemical analyses, namely dry matter (DM), organic matter (OM), crude fat (CF), crude protein (CP), neutral detergent fibre (NDF), acid detergent fibre (ADF), acid detergent lignin (ADL) profiling fatty acid (FA) and phosphorus and phytic acid content. The dehydrated TPOC had only 8% moisture content (due to drying), followed by EOC with 10% and COC (65–79%). The CF content was high in COC 1 (14.5% in DM), residual in EOC (1.5%) and intermediate in TPOC (9–10%). CP ranged from 5.3 to 7.3%. Notably, NDF levels were high (>65% in 5 samples; pitted TPOC 57.4%) and very lignified (ADL > 23%). Different FA profiles were observed: COC had the highest monounsaturated (76.36 g/100 g), while EOC had the highest saturated (16.56 g/100 g) and polyunsaturated (14.14 g/100 g). Phosphorus and phytic acid content (g/100 g) of EOC 2, TPOC pitted, TPOC dehydrated, COC 1 and COC 2 showed similar values to each other (mean of 0.12 ± 0.02 and 0.44 ± 0.0, respectively), with EOC 1 having the lowest levels (0.07 ± 0.01 and 0.26 ± 0.04, respectively). These results highlight the potential of OCs, especially dry TPOC, which offers transport, conservation and utilisation benefits.