Provided are a computer program product, system, and method for using trap cache segments to detect malicious processes. A trap cache segment to the cache for data in the storage and indicated as a trap cache segment. Cache segments are added to the cache having data from the storage that are not indicated as trap cache segments. A memory function call from a process executing in the computer system reads data from a region of a memory device to output the read data to a buffer of the memory device. A determination is made as to whether the region of the memory device includes the trap cache segment. The memory function call is blocked and the process is treated as a potentially malicious process in response to determining that the region includes the trap cache segment.