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In this article we describe and discuss means that foster the emergence of innovation through representational methods which interrelate manual modeling with playfulness. Based on the observation that demands to innovation processes have changed significantly in recent years due to changed collaboration forms, like co‐configuration or open innovation, we look for a methodological approach able to deal with such collaboration forms. We describe and discuss a methodological approach on how innovation processes in heterogeneous – interdisciplinary, cross‐functional and interorganizational – groups can be kicked off to bring about collectively shared understanding, as well as the ability to develop creative ideas. The approach relies on a playful modeling methodology, which is based on the hands‐on creation of visualizations and physical models in connection with their verbal explanation and narration. With reference to two case studies we report and discuss experiences of applying the methodology.

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SESAMI, a comprehensive program for the elucidation of the structure of complex compounds of carbon, incorporates a structure reduction-based structure genearator (COCOA). Observed limitations with this program in the solution of higher molecular weight unknowns prompted the development of a structure generator (HOUDINI) which embodies a new concept, convergent structure generation. A comparison of the performance of COCOA-based and HOUDINI-based SESAMI using a set of complex, naturally occurring compounds as a test set of unknowns revealed faster execution times and more efficient processing of ambiguous structural information for the latter.