As　energy　currency　of　life,　adenosine　triphosphate　(ATP)　is　highly　dynamic　in　living　organisms.　It　is　crucial　yet　challenging　to　probe　intracellular　or　in-vivo　ATP　precisely　without　destruction　of　the　living　biological　systems.　Herein,　we　have　designed　novel　ATP-responsive　ratiometric　nanoprobes　by　employing　upconversion　nanoparticles　(UCNPs)　with　cypate　as　antennas.　Nuclear　magnetic　resonance　spectroscopy　was　used　to　analyze　the　interfacial　interactions　among　lanthanide　nanocrystal,　cypate　and　adenosine　phosphates,　disclosing　the　origin　of　detection　specificity.　ATP　induced　interruption　of　energy　transfer　pathway　in　cypate-sensitized　UCNPs　was　further　investigated　by　femtosecond　transient　absorption　and　time-resolved　photoluminescence　spectroscopy.　The　nanoprobes　with　dual　near-infrared　(NIR)-excited　ratiometric　UCL　were　successfully　applied　for　quantification　of　ATP　level　in　living　cells　under　vegetatively　growing,　starving,　and　glycolysis-inhibiting　states,　respectively.　Furthermore,　the　increase　of　available　energy　by　feeding　for　zebrafish　larvae　was　confirmed　through　monitoring　the　in-vivo　ATP　variation　with　the　nanoprobes.　Such　nanoprobes　showed　great　potential　in　ATP-associated　biological　research　and　clinical　applications.　These　findings　may　gain　deep　insights　into　the　surface　science　and　photophysics　in　dye-lanthanide　nanocomposites,　and　open　new　avenues　for　the　design　and　bioapplications　of　lanthanide　nanoprobes.