The fascinating, complex behavior of ionic liquids is analyzed using a molecular perspective that emphasizes the doubly dual nature of ionic liquids underlying the existence of cations and anions forming high- and low-charge-density regions. Our work bridges the liquid, gas, and solid phases spanning 5 years of research on themes as diverse as the vaporization, liquid-liquid demixing, solidification, and thermophysical behavior of ionic liquids and their mixtures and solutions.