The cocoa shell (CS) is being incorporated into different food products due to its recognized content of bioactive compounds. In the case of cocoa shell infusions (CSI), the bioactive compounds that manage to be transferred to the infusion have yet to be clearly known, i.e., what is really available to the consumer. In this study, CS was obtained from toasted Colombian Criollo cocoa beans. Three particle sizes (A: >710 µm; B: >425 and <710 µm; C: <425 µm) were evaluated in the CSI, which was traditionally prepared by adding CS to hot water (1%). The decrease in particle size increased the antioxidant capacity (DPPH and ABTS) and the total phenolic compounds. A significant effect (p< 0.05) both of the particle size and of the temperature of tasting was found on some sensory attributes: greater bitterness, acidity, and astringency were due to the greater presence of epicatechin, melanoidins, and proanthocyanidins in the smaller particle sizes. The analysis of the volatile organic compounds showed that the CSI aroma was characterized by the presence of nonanal, 2-nonanone, tetramethylpyrazine, α-limonene, and linalool, which present few variations among the particle sizes. Moreover, analysis of biogenic amines, ochratoxin A, and microbial load showed that CSI is not a risk to public health. Reducing particle size becomes an important step to valorize the functional properties of CS and increase the quality of CSI.