For people with severe or profound intellectual disability (ID), support staff are important interaction partners. The quality of their interactions, a multidimensional construct, is well documented, but the staff perspective remains underexposed. This study aims to capture the behaviors, thoughts, and emotions of staff when interacting with their clients, and their views on what constitutes quality. Thirty-four support staff completed a 5-day diary about a daily interaction with a specific client. A thematic analysis was carried out. The diary entries depicted behaviors and thoughts with different foci, and emotions with positive and negative valences. The pursuit of Harmonization and the experience of Return emerged as overarching dimensions central to staff’s views on quality interaction. Limitations and directions for future research are discussed.