Inactive behavior is common in hospitalized patients. This study investigated the effectiveness of using a smartphone app with an accelerometer (Hospital Fit) in addition to usual care physiotherapy on increasing patients’ physical activity (PA) behavior. A randomized controlled trial was performed at Maastricht University Medical Centre. Patients receiving physiotherapy while hospitalized at the department of Pulmonology or Internal Medicine were randomized to usual care physiotherapy or using Hospital Fit additionally. Daily time spent walking, standing, and upright (standing/walking) (min) and daily number of postural transitions were measured with an accelerometer between the first and last treatment. Multiple linear regression analysis was performed to determine the association between PA behavior and Hospital Fit use, corrected for functional independence (mILAS). Seventy-eight patients were included with a median (IQR) age of 63 (56–68) years. Although no significant effects were found, a trend was seen in favor of Hospital Fit. Effects increased with length of use. Corrected for functional independence, Hospital Fit use resulted in an average increase of 27.4 min (95% CI: −2.4–57.3) standing/walking on day five and 29.2 min (95% CI: −6.4–64.7) on day six compared to usual care. Hospital Fit appears valuable in increasing PA in functionally independent patients.