Inking by marine molluscs such as sea hares, cuttlefish, squid, and octopuses is a striking behavior that is ideal for neuroecological explorations. While inking is generally thought to be used in active defense against predators, experimental evidence for this view is either scant or lacks mechanistic explanations. Does ink act through the visual or chemical modality? If inking is a chemical defense, how does it function and how does it affect the chemosensory systems of predators? Does it facilitate escape not only by acting directly on predators but also by being an alarm signal for conspecifics? This review examines these issues, within a broader context of passive and active chemical defensive secretions. It focuses on recent work on mechanisms of defense by inking in sea hares (Aplysia) and extends what we have learned about sea hares to other molluscs including the cephalopods.