Purpose: We aimed to investigate the benefit of a screening tool in selecting head-injured children who can potentially cooperate with computed tomography (CT). Methods: The study population consisted of head-injured children aged 36 months or younger who visited the emergency department (ED) and underwent CT from January 2013 through December 2020. Procedural sedation and analgesia (PSA) using per os chloral hydrate or per rectal thiopental was implemented to children presumed less cooperative for CT as per a clinical screening tool for cooperative candidates for CT (e.g., ability to lie still on bed for 10 seconds without a guardian). According to the PSA and the first attempt success of CT, we compared baseline characteristics, CT findings, clinically important traumatic brain injury, ED length of stay (EDLOS), and ED disposition. Results: Among the 247 children, PSA was used in 102 (41.3%). The PSA group showed a higher proportion of 3-36 months of age (PSA, 96.1% vs. non-PSA, 82.8%; P = 0.001) and longer median EDLOS (PSA, 127.0 [interquartile range, 101.0-172.0] vs. non-PSA, 85.0 minutes [63.0-130.0]; P < 0.001). The number of children undergoing the first attempt success was 213 (86.2%) without a difference in both groups (PSA, 84.3% vs. non-PSA, 87.6%; P = 0.645). In the 213 children, the implementation of PSA was associated with longer median EDLOS (PSA, 121.0 [99.0-156.0] vs. non-PSA, 77.0 minutes [60.0-122.0]; P < 0.001). In the non-PSA group (n = 145), the first attempt failure was associated with the presence of skull fracture (success, 7.1% vs. failure, 27.8%; P = 0.009). Conclusion This study suggests a potential benefit of the screening tool in selecting cooperative candidates for CT, i.e., those who could forgo PSA using oral chloral hydrate or per rectal thiopental, in young children with head injury.