Abstract: N-Methylol derivatives of herbicidal 4-amino-1,2,4-triazine-5-ones can be prepared by reacting formaldehyde with a 4-amino-1,2,4-triazine-5-one slurried in water under basic conditions. The N-methylol derivatives can be surface-modified by slurrying particles of the derivatives in water and treating with a strong acid or strong base, producing a product that releases the original herbicidal 4-amino-1,2,4-triazine-5-one in a controlled manner.