The intracellular microenvironment involves vital physiological characteristics of various cellular compartments. The fabrication of nanoprobes for subcellular measurement is important to fully characterize cellular function. Single-cell interrogation at the nanoscale is carried out mainly via optical approaches, such as the use of fluorescent dyes,1–3 quantum dots or nanoparticles,4–11 nanofiber probes,12,13 single nanowire probes,14–19 and planar photonic crystal nanowaveguides;20 mechanical approaches, such as the use of atomic force microscopy probes21–23 and nanobeam arrays;24 and electrochemical approaches, such as the utilization of single metal nanowires,25,26 pillars, or tube electrodes.27–31 Dyes and quantum-dot-based probes have attracted much attention in biology, attributable to their photoluminescence (PL), and achieved great success in measuring the temperature of cells and their organelles,32,33 as they can be easily phagocytosed by cells due to their ultrasmall dimensions and are quite robust against external disturbances. However, these techniques suffer from some limitations, such as fluorescence bleaching and background fluorescence interruption. Optical nanofibers have become increasingly popular owing to their excellent optical waveguiding property, high flexibility, and ease of integration34 and thus have been applied for the detection of intracellular pH14 and ionic concentrations.15 Notably, the existing fiber probes are passive in nature and serve only as conduits to guide light signals into/from a cell but not as a complete optical functional module for physical or chemical label-free sensing. Accordingly, most nanoprobe techniques still have to modify other nanoparticles, resulting in the low functional integration of structures.