Due to the escalating demand for conventional potassium sources, and their unavailability in many African countries, there is a growing interest in hydrothermally treated igneous rocks as viable alternatives. These materials exhibit promising potential in enhancing potassium release, comparable to traditional sources like muriate of potash (M.O.P.). However, it remains uncertain whether they can adequately fulfill the nutrient requirements of plants. In this study, we evaluated nutrient balance in ryegrass (Lolium multiflorum) using raw and hydrothermally treated K-bearing silicate rocks as fertilizers. The Compositional Nutrient Diagnostic (CND) approach was used to assess the plants’ nutrient status, involving identification of high-yield subpopulations, and setting a yield cutoff. We derived a theoretical threshold for nutrient imbalance (CNDr2) using statistical methods like the chi-square distribution function and low-yield subpopulation proportion. CNDr2 was validated via Cate–Nelson partition and sum of squared individual nutrient indexes. Results showed a yield cutoff of 37.759 kg ha−1, distinguishing low-yield and high-yield subpopulations based on cumulative variance ratio functions from survey data. The theoretical threshold derived using the chi-square function was 10.1, subsequently validated by the Cate–Nelson method. Critical CND nutrient indices were symmetrical around zero, but their sum indicated foliar nutrient imbalance, notably zinc, potassium, and copper excess, attributed to 20 interactions identified (4 synergetic and 16 antagonistic). This study underscores hydrothermal treatment’s efficacy in improving nutrient availability and achieving a balanced nutrient profile compared to raw materials. It offers a promising solution for enhancing agricultural productivity, especially in tropical regions like Africa, where traditional sources are scarce.