This PDF file includes:

• Supplementary Materials and Methods
• fig. S1. Calibration curve for the surface coverage of PLL-PEG-bio.
• fig. S2. Phase transition of the DNA-functionalized PS spheres.
• fig. S3. Schematics of the oil-water interface.
• fig. S4. Microrheology on the oil-water interface.
• fig. S5. Schematic representation of the stochastic model.
• fig. S6. Dependence of the binding density on the flux and diffusion coefficient.
• fig. S7. Pairwise potential for different strengths AO potential.
• table S1. Various DNA constructs used in the experiments.
• Reference (42)

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Other Supplementary Material for this manuscript includes the following:

• video S1 (.avi format). Dynamics of DNA-anchored colloids in gas phase imaged with 30 frames/s, focusing on the south pole.
• video S2 (.avi format). Dynamics of colloids aggregated into 2D crystals on OD surfaces imaged with 5 frames/s, focusing on the south pole.
• video S3 (.avi format). Single 1-μm large colloids DNA-anchored to the OD imaged with 50 frames/s.
• video S4 (.avi format). Single 1-μm large colloid diffusing freely in solution (kept in focus with a feedback mechanism), imaged with 50 frames/s.