Amylose content (AC) and percentage of chalkiness (PC) are the two most important quality parameters of rice (Oryza sativa L.). Breeding for high-quality medium-grain rice has been a decisive demand for the current market and consumption. This research aimed to study the crossing populations and the selection of early generations of promising combinations for evaluation in the next generations. The crossing populations’ assessment ensued for genetic variability (PCV and GCV), heritability (h2BS), and genetic advance (GAM) for the related traits. The promising rice population’s election for pure lines employed marker-assisted selection (MAS). The result showed three promising maternal cultivars (PY2, Sieu Ham Chau, and ML202) and paternal cultivars (M-202, Saturn, and Palmyra). Through the analysis of genetic parameters in the rice F2 populations, the cross combination of ML202/M-202 was the choice because of its valuable genetic parameters expected with PCV and GCV ≥ 20%, h2BS ≥ 60%, and GAM ≥ 20% for both traits of AC and PC. The Chi-square test of the variables AC and PC in the cross-population ML202/M-202 indicated the segregated ratios of 3:1 in the phenotype and 1:2:1 in the genotype. Applying MAS to select the promising rice F2 populations resulted in 92 individuals carrying genes identified with low AC and PC simultaneously. These individual rice genotypes became options for evaluation in the next generations.