The aim of this study was to analyze how motivation and classroom social climate was enhanced in the teaching–learning context throughout a Pedagogical Model of Personal and Social Responsibility (TPSR) implementation using a mixed method approach. An educational program was applied during an academic year in a student sample of primary and secondary school. A total of 44 sessions with 54 participants, between 11 and 16 years old (M = 13.41 years, SD = 1.73) were video-recorded. A multilevel triangulation design of mixed method research was applied to merge: (a) the Observational System of Teaching Oriented Responsibility (OSTOR), which revealed how the students’ behavior patterns shifted an alongside the interventions with (b) a set of five complementary questionnaires: Motivation toward Education Scale (EME), Responsibility Questionnaire (PSRQ), Basic Psychological Needs Questionnaire (PNSE), Questionnaire to assess social school climate (CECSCE) and Questionnaire of School Violence (CUVE). The mixed methods design confirmed that both the observational and the inferential analysis show an improvement of the TPSR implementation in the student’s responsibility and satisfaction and the social climate of the classroom. The other variables, although they were also improved, did not do it significantly; all the motivation dimensions showed higher values, except for amotivation and violence.