Background: Post-hemicraniectomy patients often need extended intensive care treatment. While computed tomography (CT) is considered the gold standard for regular imaging, its frequent use could be linked to adverse clinical outcomes. This study aimed to assess bedside transcranial ultrasound (TUS) to capture intracranial anatomical structures and pathologies. Methods: We analyzed 19 patients treated in our neurosurgical ICU from 1 January 2023 to 1 February 2024. Six physicians from our unit (three residents and three attending physicians) conducted a retrospective evaluation. A total of 158 sessions, including multiple freeze frames and video footage, were analyzed, including 7 imaging categories, using a Likert scale. Subsequently, correlation between CT and TUS was evaluated for midline (ML) shift, subdural space, lateral ventricular width (LVW), and extent of intracerebral hematoma using the Pearson’s correlation coefficient (r). Results: TUS was performed on average on 8.32/19.53 days (mean inpatient stay). It provided the lowest Likert scores for the imaging categories ventricular system, midline, subdural space, intraventricular catheter placement, and cortical gyration. Residents reported slightly inferior assessability, resulting in higher scores on the Likert scale (0.02–0.93 mean difference compared with attending physicians). A high correlation was shown in terms of ML shift, LVW, and intracerebral hematomas. No relevant correlation was shown in subdural space. Conclusions: TUS is a safe, cost-, and time-efficient method, potentially gaining relevance for imaging post-hemicraniectomy patients. In our setting, the method seemed effective in depicting intraventricular catheter placement, hydrocephalus, ML shift, and space-occupying lesions. Further improvement in image quality could potentially reduce the overall number of indicated CT scans.