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Herein, we report an \u201call\u2010nucleotide\u201d platform that spontaneously condenses into hierarchically organized G\u2010quadruplex (G4)\u2010based supramolecular networks and hydrogels with intrinsic biocatalytic activity. Co\u2010assembly of guanosine 5\u2032\u2010monophosphate (GMP) with adenosine phosphate derivatives reveals that phosphate multiplicity and intrinsic acidity cooperatively govern hierarchical self\u2010assembly. While adenosine monophosphate (AMP) exhibits limited organization, adenosine di\u2010 and triphosphates (ADP and ATP) drive a concentration\u2010dependent transition from liquid\u2010liquid phase\u2010separated intermediates to fibrillar networks, with GMP as the primary structural building block. Multivalent phosphate interactions and local pH modulation regulate charge screening and proton redistribution, promoting G\u2010quartet stacking. ADP affords superior structural organization due to optimal alignment within a favorable pH window. At higher concentrations, both ADP\u2010GMP and ATP\u2010GMP systems form stable, self\u2010supporting hydrogels. These hydrogels act as efficient, metal\u2010free peroxidase mimics with enhanced substrate affinity compared to native horseradish peroxidase (HRP), while also serving as confined microenvironments for enzyme encapsulation, supporting multi\u2010step cascade reactions and sensitive biomolecule detection. This work establishes a minimalistic strategy integrating biomolecular condensation with catalysis for artificial microreactors, biocatalysis, and protocell\u2010inspired materials.<\/jats:p>","DOI":"10.1002\/chem.71444","type":"journal-article","created":{"date-parts":[[2026,7,29]],"date-time":"2026-07-29T12:36:26Z","timestamp":1785328586000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Enzyme\u2010Mimicking \u201cAll\u2010Nucleotide\u201d G\u2010Quadruplex Hydrogel as a Dual\u2010Function Microreactor for Biomimetic Cascade Catalysis"],"prefix":"10.1002","author":[{"given":"Suryakamal","family":"Sarma","sequence":"first","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Indore  Indore Madhya Pradesh India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Divyanshi","family":"Deshwal","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indian 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