Grounded in Vroom’s motivational framework of performance, we examine the interactive influence of collective human capital (ability) and aggregated service orientation (motivation) on the cross-level relationship between high-performance work systems (HPWS) and individual-level service quality. Results of hierarchical linear modeling (HLM) revealed that HPWS related to collective human capital and aggregated service orientation, which in turn related to individual-level service quality. Furthermore, both HLM and ordinary least squares regression analyses revealed a cross-level interaction effect of collective human capital and aggregated service orientation such that high levels of collective human capital and aggregated service orientation influence individual-level service quality.