Resumen: Recent work has shown that nanoparticles can be ordered in semicrystalline polymers by controlling the crystallization rate, specifically by forcing them to migrate to the amorphous regions of the lamellar morphology. Here, we study the micromechanical behavior of neat polyethylene and silica/polyethylene nanocomposites filled with 15 nm brush-modified silica in the quenched and slow-crystallized organized state. The molecular response to loading in tension was monitored with Raman spectroscopy using the peaks associated with crystalline and amorphous regions. The addition of nanofillers dramatically reduced the shift in the amorphous peaks, indicating that in addition to carrying some load, the brush-modified nanoparticles may be acting as tie molecules that restrict amorphous deformation. The higher degree of lamellar organization and the organization of the nanoparticles also impacted the crystalline peak shifts, but more subtly. Idioma: Inglés DOI: 10.1080/20550324.2025.2471679 Año: 2025 Publicado en: Nanocomposites 11, 1 (2025), 68-78 ISSN: 2055-0324 Tipo y forma: Article (Published version) Área (Departamento): Área Ingeniería Química (Dpto. Ing.Quím.Tecnol.Med.Amb.)