Nuclear magnetic resonance (NMR) relaxometry techniques have been widely used for evaluating hydrated cement paste as non-destructive and quantitative measurements. The important crystalline solid phases, such as Portlandite and Ettringite, are formed in the hydration of cement paste. However, it is challenging to quantify these crystalline solid phases by conventional NMR relaxation methods, due to their short-lived NMR signal lifetimes. A novel method for 2-D NMR <inline-formula xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"> <tex-math notation="LaTeX">$T_{1}$ </tex-math></inline-formula> – <inline-formula xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"> <tex-math notation="LaTeX">$T_{\mathrm {2S}}$ </tex-math></inline-formula> measurement of hydrated cement paste is proposed in this article. Combining a homebuilt NMR probe with short deadtime and high sensitivity, the <inline-formula xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"> <tex-math notation="LaTeX">$T_{1}$ </tex-math></inline-formula> – <inline-formula xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"> <tex-math notation="LaTeX">$T_{\mathrm {2S}}$ </tex-math></inline-formula> method can provide a more complete assessment of hydrogen-bearing crystalline solid phases (i.e., Portlandite and Ettringite) in hydrated cement paste. Experimental results demonstrated that the proposed method produced two additional distinct peaks in the <inline-formula xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"> <tex-math notation="LaTeX">$T_{1}$ </tex-math></inline-formula> – <inline-formula xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"> <tex-math notation="LaTeX">$T_{2}$ </tex-math></inline-formula> correlation map, compared with conventional methodologies. The attribution of the two peaks to Portlandite and Ettringite in hydrated cement paste was confirmed by heating experiments and partial least-square regression (PLSR) method. This technique has enabled detection and quantification of Portlandite and Ettringite in hydrated cement paste.