Due to their complex and fluctuating needs requiring multiple transitions of care through different services and systems, the early postdischarge period is one of the vulnerabilities for people with acquired neurological disability. This study aimed to (1) map and examine system-level care transitions, including change in transition patterns and service use among people with acquired neurological disability during the first 12 months postdischarge and (2) explore the relationship between early perceptions (3 months postdischarge) of obstacles and difficulty with health service access to the pattern of care transitions. From July 2019 to March 2020, this study recruited 93 participants with acquired neurological disability resulting from acquired brain (44%) or spinal cord injury (56%) from a tertiary hospital in Queensland, Australia. Data linkage methods were used to capture system-level care transitions as movements between three levels of health care: primary, specialist, and emergency care. Health service use during care transitions was also characterised. Standardised questionnaires were used to measure obstacles and difficulty accessing health services in relation to transportation, finance, and resource availability at 3 months postdischarge. The median number of care transitions was 8 (range: 0–47), and the most frequent category of care transition pattern was where participants transit between all levels of care: primary, specialist, and emergency (n = 51/93, 54.8%). However, the frequency, direction, and sequence of transitions between different levels of care were diverse amongst participants. Most participants used primary (96%) and specialist (97%) services, while 59% used emergency services. Overall, postdischarge care transitions were common and highly variable for people with acquired neurological disability. Early perceptions of transportation being an obstacle to service access was a marginally significant contributor (p = 0.051) to more care transitions. Further research to delineate the characteristics and complications of care transitions and service use will aid in developing more personalised, coordinated postdischarge trajectories.