The aims of this study were to identify the most needed health care services, accessibility of various health care services, and barriers to access as perceived by a group of Syrian refugees living in non-camp settings in Jordan and to compare accessibility among different groups. The study was conducted in the Amman, Irbid, Karak, and Maan governorates of Jordan. This is a cross-sectional, analytical, observational study using convenience and snowball sampling for data collection. A structured questionnaire was included in an ongoing needs assessment of a Jordanian nongovernment organization in April 2014, with a total of 196 surveys conducted. In addition to the prevalent acute and communicable diseases, chronic diseases and dental problems were common. Preventive and primary health care were more accessible than advanced services. Structural and financial barriers hindered access. The specific survey location and governorate were associated with a difference in reported access. Registration status, health provider, duration, and out-of-pocket payment did not affect accessibility. The capacities of health facilities at different levels should be increased. Enhanced information sharing among health providers can improve identification of needs and gaps.