NMR Relaxation (NMRR) is an extremely useful quantitative technique for material science, particularly for studying polymers and porous materials. NMR Cryoporometry (NMRC) is a powerful technique for the measurement of pore-size distributions and total porosities. This paper discusses the use, capabilities and application of a newly developed compact NMR time-domain relaxation spectrometer suitable for studying both solid and liquid samples (Mk3 NMR Relaxation spectrometer & Cryoporometer, Lab-Tools (nano-science), Ramsgate, Kent, UK. (2019)). This highly compact precision NMR Spectrometer is based on a Field Programmable Gate array (FPGA) module and custom surface mount low-noise NMR receiver and NMR linear transmitter. A high proportion of the RF circuitry is in a digital form, implemented as firmware in the FPGA, which gives the instrument an excellent long-term stability. It also includes an on-chip Linux computer. The FPGA module is credit-card sized, and both the NMR receiver and NMR transmitter are even smaller. The software, including the top-level NMR pulse sequence definitions, are written in an array processing language, Apl. The spectrometer comes complete with a Graphical User Interface (GUI) for control and on- and offline curve fitting and data analysis. The recent development of the Lab-Tools Peltier thermo-electrically cooled NMR variable-temperature (V-T) probe that cools the sample below −60 °C is also discussed. This Peltier cooling gives the precision temperature control and smoothness needed by NMR Cryoporometry (10 mK near the probe liquid bulk melting point). This enables the NMRC measurement of pore-size distributions in porous materials, for the unusually wide pore-size range of sub-nano to over 1 micron-sized pores. The NMR Spectrometer’s unusually small size, ability to measure solids, low noise and high performance make it particularly suitable for material science studies both in the field and in university, research institute, company and even school laboratories. A human portable version now exists. Use of the controlling GUI is described, and results from example NMR Relaxation and NMR Cryoporometric measurements are given.