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PLLA chains crystallize into diamond\u2010shaped platelets in isopropanol, which forces the terminal dyes to assemble into a 2D array on the platelet surface by either dipolar interactions or \u03c0\u2010stacking and exhibit tunable emission. Dipolar dyes play a critical role in imparting colloidal stability and structural uniformity to the 2D crystals, which is partly compromised for hydrophobic ones. Co\u2010crystallization between NMI\u2010 and PY\u2010labeled PLLAs yields similar diamond\u2010shaped co\u2010platelets with highly efficient (\u224880\u2009%) F\u00f6rster Resonance Energy Transfer on the 2D surface. 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