Herbert wrote poetry in English, Latin and Greek. In 1633 all of Herbert's English poems were published in The Temple: Sacred Poems and Private Ejaculations, with a preface by Nicholas Ferrar. The book went through eight editions by 1690. According to Walton, when Herbert sent the manuscript to Ferrar, he said that "he shall find in it a picture of the many spiritual conflicts that have passed between God and my soul, before I could subject mine to the will of Jesus, my Master". The poems imitate the architectural style of churches through both the meaning of the words and their visual layout. Herbert used the very format of the poems to reinforce the theme he was trying to portray. The themes of God and love are treated by Herbert as psychological forces as much as metaphysical phenomena.
All of Herbert's surviving English poems are religious, and some have been used as hymns. They are characterised by directness of expression and some conceits which can appear quaint. Many of the poems have intricate rhyme schemes, and variations of lines within stanzas; according to Helen Vendler, "a cascade of form floats through the temple". William Cowper said of them, "I found in them a strain of piety which I could not but admire". John Wesley was one of the individuals who took Herbert's lyrics and made them into hymns.
An example of Herbert’s religious poetry is “The Altar,”  a "pattern poem” in which the words form a shape on the page suggesting an altar. The altar is used as his conceit or metaphor for how the individual offer himself as a sacrifice to the Lord. Herbert also makes allusions to scripture, such as Psalm 51:17, where it states that the Lord requires the sacrifice of a broken heart and a contrite spirit.
Another example of Herbert's religious pieces is "The Windows,"  is a piece expanding upon man's incapacity to share the word of God, and the gift that it is that God allows and enabled him to do so. He compares a righteous man to a glass window, through which God's light shines.
Herbert's only prose work, A Priest to the Temple (usually known as The Country Parson), offers practical advice to rural clergy. In it, he advises that "things of ordinary use" such as ploughs, leaven, or dances, could be made to "serve for lights even of Heavenly Truths". It was first published in 1652 as part of Herbert's Remains, or Sundry Pieces of That Sweet Singer, Mr. George Herbert, edited by Barnabas Oley. The first edition was prefixed with unsigned preface by Oley, which was used as one of the sources for Izaak Walton's biography of Herbert, first published in 1670. The second edition appeared in 1671 as A Priest to the Temple or the Country Parson, with a new preface, this time signed by Oley.
Like many of his literary contemporaries, Herbert was a collector of proverbs. His Outlandish Proverbs was published in 1640, listing over 1000 aphorisms in English, but gathered from many countries (in Herbert's day, 'outlandish' meant foreign). The collection included many sayings repeated to this day, for example, "His bark is worse than his bite" and "Who is so deaf, as he that will not hear?" These and an additional 150 proverbs were included in a later collection entitled Jacula Prudentum (sometimes seen as Jacula Prudentium), dated 1651 and published in 1652 as part of Oley's Herbert's Remains.
Richard Baxter said, "Herbert speaks to God like one that really believeth a God, and whose business in the world is most with God. Heart-work and heaven-work make up his books". Dame Helen Gardner adds "head-work" because of his "intellectual vivacity".