Research in functional materials is frequently driven by a desire to make informed choices in the quest for better, more effective materials. A great deal of recent attention has been focused on the modalities of how such informed choices can themselves be made in a better, more effective manner. The examples presented here examine some of these modalities, emphasizing the nexus between new synthesis, computational design and analysis, growth in high purity forms, and finally, end-use in terms of either application or of significant property measurement. The illustrations, many drawn from the recent literature, commence with the role that theory has played, both in property prediction and concomitant materials selection, in the areas of multiferroics and topological insulators. The importance of materials quality is emphasized, using examples from observation of the fractional Quantum Hall Effect, where new science has emerged as a result of improved materials. In the area of organic electronics, prospects for advancing the field are suggested, as are future directions in nanoscience. While the examples chosen here point to developments that require a highly collaborative “systems” approach to materials, the role that serendipity plays is not ignored.