Noise pollution is an issue of high concern in urban environments and current standards and regulations trend to increase acoustic insulation requirements concerning airborne noise control. The design and development of novel building materials with enhanced acoustic performance is an efficient solution to mitigate this problem. Their application as renders and plasters can improve the acoustic conditions of existing and brand-new buildings. This paper reports the acoustic performance of eleven multiscale porous lime-cement mortars (MP-LCM) with two types of fibers (cellulose and polypropylene), gap-graded sand, and three lightweight aggregates (expanded clay, perlite, and vermiculite). Gap-graded sand was replaced by 25 and 50% of lightweight aggregates. A volume of 1.5% and 3% of cellulose fibers were added. The experimental study involved a physical characterization of properties related to mortar porous microstructure, such as apparent density, open porosity accessible to water, capillarity absorption, and water vapor permeability. Mechanical properties, such as Young’s modulus, compressibility modulus, and Poisson’s ratio were evaluated with ultrasonic pulse transmission tests. Acoustic properties, such as acoustic absorption coefficient and global index of airborne noise transmission, were measured using reduced-scale laboratory tests. The influence of mortar composition and the effects of mass, homogeneity, and stiffness on acoustic properties was assessed. Mortars with lower density, lower vapor permeability, larger open porosity, and higher Young’s and compressibility modulus showed an increase in sound insulation. The incorporation of lightweight aggregates increased sound insulation by up to 38% compared to the gap-graded sand reference mixture. Fibers slightly improved sound insulation, although a small fraction of cellulose fibers can quadruplicate noise absorption. The roughness of the exposed surface also affected sound transmission loss. A semi-quantitative multiscale model for acoustic performance, considering paste thickness, active void size, and connectivity of paste pores as key parameters, was proposed. It was observed that MP-LCM with enhanced sound insulation, slightly reduced sound absorption.