The superior mass sensitivity of micro-coil technology in Nuclear Magnetic Resonance (NMR) Spectroscopy provides potential for the analysis of extremely small mass-limited samples such as eggs, cells, and tiny organisms. For optimal performance and efficiency, the size of the micro-coil should be tailored to the size of the mass-limited sample of interest, which can be costly as mass-limited samples come in many shapes and sizes. Therefore, rapid and economic micro-coil production methods are needed. One method with great potential is 5-axis Computer Numerical Control (CNC) micro-milling, commonly used in the jewelry industry. Most CNC milling machines are designed to process larger objects and commonly have a precision >25 µm (making the machining of common spiral micro-coils, for example, impossible). Here, a 5-axis MiRA6 CNC milling machine, specifically designed for the jewelry industry, with a 0.3 µm precision was used to produce working planar micro-coils, microstrips, and novel micro-sensor designs, with some tested on the NMR in less than 24 hours after the start of the design process. Sample wells could be built into the micro-sensor and could be machined at the same time as the sensors themselves, in some cases leaving a sheet of Teflon as thin as 10 µm between the sample and sensor. This provides the freedom to produce a wide array of designs and demonstrates 5-axis CNC micro-milling as a versatile tool for the rapid prototyping of NMR micro-sensors. This approach allowed the experimental optimization of a prototype microstrip for the analysis of two intact adult Daphnia magna organisms. In addition, a 3D volume slotted tube resonator was produced that allowed for 2D 1 H-13 C NMR of D. magna neonates and exhibited 1 H sensitivity (nLOD ꙍ 600 = 1.49 nmol s 1/2 ) close to that of double striplines, which themselves offer the best compromise between concentration and mass sensitivity published to date.