在1908年夏季，勋伯格的妻子玛蒂尔德离开他数月，与一位年轻的奥地利画家里夏德·格斯特尔（英语：Richard Gerstl）（后来在玛蒂尔德回到婚姻后于同年11月自杀）发生了关系。这一时期标志着勋伯格作品的明显变化。在妻子离开期间，他创作了《你靠在一棵银柳树上》（德语：Du lehnest wider eine Silberweide），这是他改编自德国神秘主义诗人施特凡·格奥尔格同名诗集的套曲《悬园之书（英语：The Book of the Hanging Gardens）》（德语：Das Buch der hängenden Gärten，作品15）中的第13首。这是他的第一首完全没有调参照的作品。[10]
第一次世界大战给他的发展带来了危机。当他42岁时，兵役打乱了他的生活。他无法持续、不受打扰地工作，结果留下了许多未完成的作品和未发展的“开端”。有一次，一位上级军官问他是否“就是臭名昭著的勋伯格”，勋伯格回答说：“报告，先生，是的。没有人想要成为他，有人必须成为他，所以我成了他。”[12]据诺曼·莱布雷希特说，这是指勋伯格作为“不和谐的解放（英语：Emancipation of the dissonance）者”的明显“命运”。[13]
当代作曲家与公众之间关系的恶化导致他在1918年在维也纳成立了私人音乐演出协会（德语：Verein für musikalische Privataufführungen）。他试图提供一个论坛，以便现代音乐作品能够经过精心准备和排练，并在受到时尚和商业压力影响的条件下仍得到适当的演出。从成立到1921年因经济原因结束为止，该协会向付费会员呈现了353场演出，有时每周一场。在最初的一年半中，勋伯格没有让自己的任何作品被演出。[15]协会音乐会的听众而是听到了斯克里亚宾、德彪西、马勒、韦伯恩、贝尔格、雷格等20世纪音乐早期的重要人物的复杂当代作品。[16]
在这一最后时期，他创作了几部重要的作品，包括小提琴协奏曲（作品36号，1934/36年）、为合唱和管弦乐团而作的《誓约》（Kol Nidre，作品39号，1938年）、《拿破仑·波拿巴颂》（Ode to Napoleon Buonaparte，作品41号，1942年）、钢琴协奏曲（英语：Piano Concerto (Schoenberg)）（作品42号，1942年），以及献给大屠杀受害者的纪念作品《华沙幸存者（英语：A Survivor from Warsaw）》（作品46号，1947年）。他未能完成自己的歌剧《摩西与亚伦》（1932/33年），该作品是最早完全采用十二音技法创作的歌剧之一。除了十二音音乐，勋伯格在最后一个时期还回归了调性，创作了G大调弦乐组曲（1935年）、降E小调第2号室内交响曲（英语：Chamber Symphony No. 2 (Schoenberg)）（作品38号，始于1906年，于1939年完成）、D小调宣叙调变奏曲（作品40号，1941年）。在这个时期，他的著名学生包括约翰·凯奇和卢·哈里森。
在1920年代初，勋伯格致力于发展一种能够使音乐织体更简单、更清晰的秩序方式。这导致了“以只与彼此相关的十二个音符进行作曲的方法”[48]，其中八度音阶内的十二个音高（在作曲中并未实现）被视为相等，没有任何一个音符或音调被赋予古典和声中所占据的重要性。他认为这一理论的重要性等同于物理中阿尔伯特·爱因斯坦的相对论的地位。勋伯格在与朋友约瑟夫·鲁费尔（英语：Josef Rufer）散步时以他典型的方式宣布了这一发现，当时他说：“我已经做出了一个发现，它将确保德国音乐在未来一百年中仍占主导地位。”[49]这个时期的作品包括《为乐团而作的变奏曲》（作品31号，1928年）；伴奏音乐《电影场景配乐（英语：Begleitungsmusik zu einer Lichtspielscene）》（作品34，1930年）；《钢琴作品》（作品Op. 33a/b号，1931年）以及钢琴协奏曲（作品42号，1942年）。人们普遍认为勋伯格作曲方法严谨，但他对这种技巧的使用因每个独立作品的要求而各不相同。因此，他未完成的歌剧《摩西与亚伦》的结构与他的《为小提琴与钢琴而作的幻想曲》（作品47号，1949年）不同。
“《政治、宗教和文化利益周刊》（德语：Wochenschrift für politische, religiöse und Cultur-Interessen）刊登了通告《来自布拉格的保琳·纳霍德小姐与来自普雷斯堡的塞缪尔·勋伯格的婚礼》。这些信息与宗教社区发布的公告不符：1872年3月17日，12时30分，塞缪尔·勋伯格，来自塞切尼的商人，亚伯拉罕先生和特丽西娅女士的儿子，出生于1838年9月15日，住址为塔博尔街4号；保琳·纳霍德，来自普雷斯堡，约瑟夫先生和卡罗琳娜女士的女儿，出生于1843年3月8日，住址为塔博尔街4号。宣布姻缘并代表出席的是普雷斯堡的代表，日期是1872年3月2日。”
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