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This study investigates the role of entrepreneurial attitudes for small and medium‐sized enterprise managers' tendency to create knowledge acquisition ties with managers of other organizations in the context of an institutionalized high‐tech cluster. We examine how innovation orientation, perceived personal control, need for achievement, and self‐esteem influence boundary‐spanning tie creation as a crucial facet of entrepreneurial behavior in the cluster context. Applying exponential random graph models to survey data collected in a German biotech cluster, we find that innovation orientation and perceived personal control positively affect managers' tendency to rely on interpersonal ties to gather knowledge. In contrast, need for achievement and self‐esteem are negatively related to knowledge tie creation.