1903359(1of31)©2020TheAuthors.PublishedbyWILEY-VCHVerlagGmbH&Co.KGaA,Weinheimwww.advancedscience.comReviewCell-InspiredAll-AqueousMicrofluidics:FromIntracellularLiquid–LiquidPhaseSeparationtowardAdvancedBiomaterialsQingmingMa,*YangSong,*WentaoSun,JieCao,HaoYuan,XinyuWang,YongSun,*andHoCheungShum*DOI:10.1002/advs.2019033591.IntroductionNaturehasevolvedforbillionsofyearstodevelopelaborateandsophisticatedlivingorganisms,[1–9]whichcanprovidesourcesofinspiredsolutionsforvariousintriguingandenduringscientificandtechniquequestions.[10–13]Althoughasinglecellisthesimplestunitoflivingorganisms,itisrichinhighdegreesofstructuralandfunctionalcomplexities.[14–17]Theamazingandvitalroleofcellsinlifehaveattractedgreatscientificinterestsforconstructing“artificialcells”bycombiningbiologicalornonbiologicalcomponentstoformmicro-scaledassembliesthatareintendedtomimiconeormoreaspectsofcells,[18–22]suchasthesemipermeablemembraneassemblyandtheabilitytoperformasimplereactionintheirinteriors.[23–26]Thedevelopmentofartificialcellularsystemshasledtoprogressesinunderstandingtheoriginoflife,connectingthenonlivingtoLivingcellshaveevolvedoverbillionsofyearstodevelopstructuralandfunctionalcomplexitywithnumerousintracellularcompartmentsthatareformedduetoliquid–liquidphaseseparation(LLPS).DiscoveryoftheamazingandvitalrolesofcellsinlifehassparkedtremendouseffortstoinvestigateandreplicatetheintracellularLLPS.Amongthem,all-aqueousemulsionsareaminimalisticliquidmodelthatrecapitulatesthestructuralandfunctionalfeaturesofmembranelessorganellesandprotocells.Here,anemergingall-aqueousmicrofluidictechnologyderivedfrommicrometer-scaledmanipulationofLLPSispresented;thetechnologyenablesthestate-of-artdesignofadvancedbiomaterialswithexquisitestructuralproficiencyanddiversifiedbiologicalfunctions.Moreover,avarietyofemergingbiomedicalapplications,includingencapsulationanddeliveryofbioactivegradients,fabricationofartificialmembranelessorganelles,aswellasprintingandassemblyofpredesignedcellpatternsandlivin...