This PDF file includes:

• Determination of the entropic contribution for hard lock and key particles
  
• Evaluation of the binding specificity
  
• fig. S1. Geometrical configuration of a particle in a lock-and-key assembly.
  
• fig. S2. Entropic contribution for hard lock and key particles.
  
• fig. S3. Binding specificity dependence of the mixing ratio between lock and key particles.
  
• fig. S4. Binding specificity dependence of the temperature at a constant mixing ratio.

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Other Supplementary Material for this manuscript includes the following:

• movie S1. (.mp4 format). Colloidal molecules with tunable valence via lock-and-key self-assembly.