Illuminated manuscripts are relatively well studied, but the available publications greatly focus on religious manuscripts of a geographically limited area. In contrast, technical examinations of illuminated legal documents have received far less attention, e.g., Spanish cartas ejecutorias de hidalguía (executory certificates of nobility). These documents are suitable case studies to deepen current knowledge of manuscript-making in Spain for two reasons: First, they are dated (late fifteenth to early eighteenth centuries); and second, they are unusual and understudied from both the textual and materials analysis standpoints. Cartas contain judicial proceedings whereby a family gained or was re-assigned hidalguía (lower nobility). A key exhibit to achieving this status was proving their “blood purity” which implied they were faithful Catholics, so finding religious representations within the document is common. In addition, families embedded their faith and links to monarchs in their coat of arms through symbols like crowned eagles, trees, and towers. The deliberate choice of heraldic and religious elements is as important as the materials used to produce them. Interested in better understanding illumination in Spain we are studying these unique documents from the historical, materials, and iconographic points of view. Herein, we present the earliest results of an ongoing survey, detailing two case studies: Davila and Nuñez D. Armesto cartas. This research uses a combination of: (a) instrumental techniques (X-ray fluorescence, reflectance, and infrared spectroscopies; peptide mass fingerprinting; and gas chromatography); and (b) historical research using both the manuscript’s contents as primary sources, and published research. The preliminary results are enabling us to shed light onto Spanish (legal) illuminated manuscript-making, and the symbolic role materials played, e.g., use of precious metals adorning monarchical elements, presence of ultramarine mixed with azurite on both coats of arms, and on Virgin Mary’s gown, etc. This survey intends to simultaneously learn more about illumination practices in Spain, inform conservation decisions, and hopefully better understand problems connected to historic ideologies that were legalized in beautiful albeit disturbing documents, e.g., persecution of non-Catholics at the time in Spain.