Most of the early Arab grammarians were chiefly concerned with the description of language structure and particularly the problem of explaining the inflectional marks. Al-Jurjānī, in the fifth century AH/eleventh century AD, was the first among Arab grammarians to depart from earlier trend of linguistic analysis and to put forward a demonstrable theory for the study of language and grammar in terms of the interrelationships that bind the constituents of speech together. According to al-Jurjānī, there are three types of relationships: syntactic relationships, semantic relationships, and the relationship between syntax and semantics. This paper contains a systematic account of these syntactic-semantic interrelationships in particular, and al-Jurjānī’s approach and methodology to language and grammar in general. Our investigation is based on an intensive study of the concepts of naẓm (discourse arrangement) and ta^clīq (interrelationship) which al-Jurjānī discussed with ample evidence and cogent reasoning in his major work Dalā’il al-I^cjāz (Illustrations of the Inimitability [of the Qur’ān]). A distinctive feature of this research is the effort made to show the connection between al-Jurjānī’s linguistic concepts and equivalent notions used in modern linguistics. The study concludes with an important fact; namely, that al-Jurjānī was one of the frontier scholars to call for the study of language on the basis of syntactic-semantic functions and as a discipline independent of grammatical regents.